bims-enlima Biomed News
on Engineered living materials
Issue of 2026–06–21
fifteen papers selected by
Rahul Kumar, Tallinna Tehnikaülikool
  1. Towards supramolecular regenerative medicine using low-molecular-weight gelator hydrogels for stem cell growth.
  2. In situ rheological monitoring of diffusion-controlled hydrogel crosslinking for embedded 3D bioprinting.
  3. Programmed synthesis of mesoporous protein crystals in cellular reactors.
  4. Programming Nonlinear Interfacial Mechanics of Synthetic Cells: Lipid Geometry and DNA Nanostructures.
  5. Hierarchical stabilization of bioactive hydrogels by multi-arm peptide-polymer supramolecular staples.
  6. Formation of assembloids by DNA-mediated synthetic cell self-assembly.
  7. Efficient prime editing in vivo and in vitro using lipid nanoparticles.
  8. Mycoelectronics: Bioprinted living fungal bioelectronics for artificial sensation.
  9. Collapsible scissored surfaces.
  10. Bioinspired design of hierarchical structured hydrogels with extraordinary lubrication and load-bearing capacity.
  11. Mechanically Enhanced Ultrashort Peptide Hydrogels for pH-Triggered Release.
  12. Electrical writing of multi-responsive polysaccharide hydrogel enabling integration of programmable deformation and information storage.
  13. Chemically triggered rapid degradation of tetraPEG gels cross-linked with a diacylhydrazine-containing cross-linker.
  14. Bio-Inspired Topologically Constrained, Interlocking-like Cellulose Architectures via Sacrificial Oligomer Templating.
  15. Engineering coordination bonds for bioinspired responsive polymers.
  1. Biomater Sci. 2026 Jun 18.
    Towards supramolecular regenerative medicine using low-molecular-weight gelator hydrogels for stem cell growth.
    Chayanan Tangsombun, David K Smith.
      This review explores gels that assemble from low-molecular-weight gelator (LMWG) building blocks for use in cell culture, with a focus on fibroblasts and stem cells. These LMWG hydrogels have unique potential for controlling and directing cell growth. We provide an overview of gel tunability and how careful molecular design can direct biological outcomes. The LMWG hydrogel approach to cell growth is based on reversible assembly, potentially enabling cells to be encapsulated and subsequently released. It is possible to easily formulate multiple active ingredients into LMWG hydrogels by co-assembly - a powerful strategy to create multi-functional hybrid hydrogels. Rheological properties can be tuned over orders of magnitude, with stiffness helping control properties like cell invasion or stem cell differentiation. Furthermore, gel dynamics at both molecular and network levels can control factors such as cell adhesion. By developing strategies to shape and pattern these gels, it is possible to create structured assemblies of cells or direct the growth of multi-functional biological tissues. The dynamic characteristics of these gels enables them to evolve, potentially facilitating 4D tissue engineering or the creation of materials that are both bio-instructive and bio-responsive. LMWG hydrogels have been applied both in vitro and in vivo and some are in commercial use. This critical review provides an overview of progress to date, emphasising the unique advantages of the LMWG hydrogel approach, and highlighting concepts that might unlock untapped potential, hence transforming next-generation regenerative medicine.
    DOI:  https://doi.org/10.1039/d6bm00661b
  2. Biofabrication. 2026 Jun 17.
    In situ rheological monitoring of diffusion-controlled hydrogel crosslinking for embedded 3D bioprinting.
    Fotis Christakopoulos, Audrey Shih, Stella J Chung, Carla Huerta-López, Lucia Giulia Brunel, Narelli De Paiva Narciso, Clélia Messin-Roizard, Junyi Tao, David Myung, Sarah Heilshorn, Gerald G Fuller.
      In embedded 3D bioprinting, biomaterial inks are extruded into sacrificial support baths to facilitate the fabrication of complex shapes, even from soft, liquid-like materials. Post-printing, the diffusion of small molecules into or out of the support bath can facilitate ink crosslinking to stabilize the printed structure. In these coupled reaction-diffusion systems, the rheological properties of the ink will change over time. Despite the importance of tuning the mechanical properties of these inks for biological applications, there are currently no methods to accurately predict ink stiffness over time throughout the crosslinking process. Here, we use a custom-developed magnetic stress rheometer to continuously monitor diffusion-driven crosslinking in situ. Our approach reveals how gelation kinetics depend on the thickness of the ink layer, and enables predictive estimation of mechanical evolution in these reaction-and diffusion-driven systems. With these insights, we fabricate specimens with predetermined mechanical properties and observe changes in cell phenotype as a response. These insights help inform the design of inks and timing of bioprinting protocols to achieve prints with desirable mechanical properties and further allow the fabrication of prints with patterned mechanical properties.
    Keywords:  Diffusion-enabled bioprinting; collagen; corneal epithelial cells; dynamic covalent crosslinking; dynamic hydrogels; embedded 3D printing
    DOI:  https://doi.org/10.1088/1758-5090/ae7ed3
  3. Nat Nanotechnol. 2026 Jun 15.
    Programmed synthesis of mesoporous protein crystals in cellular reactors.
    Hongru Yang, Dian-Zhao Lin, Zhe Li, Yuqing Yan, Zuo-Han Zhao, Byeongdu Lee, Chang Woo Song, Shunzhi Wang, Jiaxi Lu, Yimei Wang, Yongzhi Sun, Ken Livi, David Baker, Yayuan Liu, Dingchang Lin.
      Protein crystals are naturally derived mesoporous materials with versatile structures and physicochemical properties. Here we introduce an intracellular synthesis platform that enables controllable and programmable protein crystallization. In live cells, we show that, after initial nucleation, steady protein expression governs crystal growth, yielding predictable, tunable dynamics in live cells. Exploiting this feature, we combined HaloTag and click chemistries to achieve modular, programmable immobilization of diverse guest materials with spatial patterning down to ~100 nm resolution. We further demonstrated the sequential release of immobilized materials in physiologically relevant fluids. As a proof of concept, we programmed particles to carry human fibroblast growth factors in distinct layers, which elicited designed oscillatory Akt signalling patterns in cell culture. This work outlines a programmable method for producing mesoporous materials, with possible applications in catalysis and biomedicine.
    DOI:  https://doi.org/10.1038/s41565-026-02198-x
  4. Small Sci. 2026 Jun;6(6): e70321
    Programming Nonlinear Interfacial Mechanics of Synthetic Cells: Lipid Geometry and DNA Nanostructures.
    Kazutoshi Masuda, Miho Yanagisawa.
      Soft interfaces formed by lipid membranes are fundamental to living cells, synthetic cells, and membrane-based soft materials. However, a quantitative framework linking molecular organization with nonlinear interfacial mechanics remains elusive. Here, we establish an analytical framework that captures the nonlinear elastic response of lipid-membrane-coated synthetic cells under micropipette aspiration. Incorporating both area stretching and curvature bending enables the model to quantitatively reproduce the complete pressure-displacement response within the small-deformation regime. This approach reduces interfacial mechanics to two parameters: the in-plane area-stretching modulus and an out-of-plane bending-related term. Using this unified framework, we experimentally demonstrate that nonlinear interfacial mechanics can be programmed by altering the molecular geometry and effective dimensionality of adsorbed elements. The lipid molecular shape and curvature-dependent packing regulate in-plane stiffness, whereas DNA nanostructures, the other adsorbed element, introduce an orthogonal control axis via dimensionality: three-dimensional network architectures markedly reinforce bending resistance. Together, these results establish a general molecular design principle for programming interfacial mechanics and provide a quantitative foundation for engineering mechanically tunable synthetic cells and soft interfaces.
    DOI:  https://doi.org/10.1002/smsc.70321
  5. J Mater Chem B. 2026 Jun 10.
    Hierarchical stabilization of bioactive hydrogels by multi-arm peptide-polymer supramolecular staples.
    Somayeh Taheri, Md Shariful Islam, Riddhesh B Doshi, Jitendra Mata, Ashley K Nguyen, Juanfang Ruan, Richard D Tilley, Kristopher A Kilian.
      Supramolecular peptide hydrogels offer attractive bioactivity and dynamic mechanical behavior for three-dimensional cell culture and tissue engineering. However, their broader use is often limited by slow gelation and insufficient mechanical stability. Here, we introduce a molecular design strategy in which a tryptophan zipper pendant multiarm poly (ethylene glycol) (Trpzip-PEG) conjugate is incorporated into Trpzip nanofibrillar hydrogels to facilitate hierarchical tuning of materials properties. Trpzip peptides self-assemble into entangled nanofiber networks, while the addition of Trpzip-PEG conjugate induces reorganization of these assemblies. Electron microscopy and neutron scattering reveal more densely bundled fibers with increased microporosity and a fractal network architecture, suggesting that the conjugate acts as a supramolecular binder or "staple" coordinating nano- and micro-scale organization. These structural changes markedly accelerate gelation and increase stiffness, yield behavior, and thixotropic recovery. Importantly, the Trpzip/Trpzip-PEG supramolecular hybrid hydrogels remain cytocompatible, supporting adipose-derived stem cell adhesion, viability, and proliferation over time. Together, these findings demonstrate that Trpzip/Trpzip-PEG hybrid hydrogels offer a versatile platform for engineering mechanically robust yet bioactive soft materials for 3D cell culture, biofabrication, and regenerative medicine applications.
    DOI:  https://doi.org/10.1039/d6tb00490c
  6. Soft Matter. 2026 Jun 12.
    Formation of assembloids by DNA-mediated synthetic cell self-assembly.
    Anna Burgstaller, Erick Angel Lopez Lopez, Gyu Min Hwang, Kevin Jahnke, Oskar Staufer.
      Approaches in tissue engineering, organoid culture, and organs-on-chip have propelled the development of increasingly sophisticated in vitro models of human tissues. However, as they are formed from natural cells, it is challenging to control their molecular composition and biophysical properties, increasing variability and limiting their robustness. To overcome these limitations, we introduce a self-assembly strategy for synthetic cells that enables the formation of millimeter-sized synthetic constructs based on single synthetic cells. Specifically, we functionalize the lipid membrane of synthetic cells with cholesterol-tagged single-stranded DNA aptamers, which drive programmable intercellular adhesion through sequence-specific hybridization. This allows individual synthetic cells to interconnect into higher order 3D constructs. By varying aptamer complementarity, internal architecture with spatially distinct functional zones and tuneable mechanical properties can be encoded. Most importantly, the DNA-driven self-assembly operates directly in cell culture medium, is compatible with high-throughput microwell formats enabling scalable screening workflows and is reversible by DNA displacement. To demonstrate the biological functionality of these synthetic tissues, we incorporate T cell-stimulatory antibodies into spatially segregated tissue regions. This design mimics lymph node organization and supports infiltration of natural primary human T cells, which subsequently expand within the synthetic tissue. Together, these results establish a route to tissue-scale matrices built from synthetic cell collectives and represent a critical step toward functionally integrating living and non-living matter.
    DOI:  https://doi.org/10.1039/d6sm00119j
  7. Nat Nanotechnol. 2026 Jun 15.
    Efficient prime editing in vivo and in vitro using lipid nanoparticles.
    Allen Y Jiang, Ana Cristian, Dominique L Brooks, Emily R Feierman, Paul Z Chen, Madelynn N Whittaker, Sarah E Pierce, Holt A Sakai, Hongyu Chen, Dangliang Liu, Peyton B Randolph, Angus H Li, Alvin Hsu, Serena O Omo-Lamai, Y Allen Tao, Benista Owusu-Amo, Xiao Wang, Xiao Wang, Kiran Musunuru, David R Liu.
      Prime editing is a versatile clinical genome editing method that enables precise substitutions, small insertions and deletions at specified locations in the genomes of living systems including human cells. Although non-viral lipid nanoparticle (LNP) delivery of RNA in vivo has become a preferred method for gene editing in animals and patients, its application to complex, three-component prime editing systems has yielded low editing efficiencies. Here we developed a systematic prime editing LNP (PE-LNP) optimization platform that addresses key bottlenecks in cargo design that limit editing efficiency. This generalizable workflow yielded PE-LNPs that can achieve 49% average in vivo prime editing in the bulk mouse liver with a single dose of 2 mg kg-1. We applied our workflow to the correction of PAH R408W, a cause of phenylketonuria, in a mouse model and achieved prime editing efficiencies and serum phenylalanine levels anticipated to be curative. We also show that PE-LNPs minimize off-target editing compared with DNA delivery methods, induce only transient elevation of liver enzymes and can be dosed repeatedly to improve editing efficiencies. These PE-LNP systems provide an attractive alternative to viral delivery by offering transient expression that minimizes off-target editing, no observed long-term toxicity and high levels of non-viral in vivo liver prime editing.
    DOI:  https://doi.org/10.1038/s41565-026-02200-6
  8. Proc Natl Acad Sci U S A. 2026 Jun 30. 123(26): e2530456123
    Mycoelectronics: Bioprinted living fungal bioelectronics for artificial sensation.
    Yulu Cai, Hang Yuan, Caleb Ronders, Vittorio Mottini, Kalpana Singh, Liuxi Xing, Iha Singh, Denghao Fu, Kyla Zhao, Linux Heller, Khoi Nguyen, Bryce Waller, Tuo Wang, Gregory Bonito, Jinxing Li.
      The intelligence of the human biological system is enabled by the highly distributed sensing receptors on soft skin that can distinguish various stimulations or environmental cues, thus establishing the fundamental logic of sensing and physiological regulation or response. To replicate biological perception, biohybrid systems integrating living organisms with electronics have been developed to sense environmental cues. However, current eukaryote-based biohybrids face slow growth, strict culture needs, and short lifespans, limiting real-world use. Here, we introduce fungi-based printable "Mycoelectronics" which are created by additive bioprinting of living fungal mycelium networks onto stretchable electronics, as a practical living thermoresponsive sensory platform. This mycoelectronics approach leverages fung's capabilities for rapid biological responsiveness, cultivability with exponential growth, stability and self-healing in ambient conditions, bioprintability for scalable manufacturing, and mechanical flexibility for seamless integration with soft electronics. We show that the thermal responsiveness of the fungal network arises from intrinsic cellular processes-specifically, heat-induced vacuole remodeling and fusion, which modulate ionic transport and thus the electrical conductivity of the mycelial cells and networks, enabling a rapid response. By bridging the gap between cell biology and soft electronics, the mycoelectronics device, with a living mycelial network, functions as a thermal sensation system with rapid response and intrinsic self-healing properties, autonomously restoring sensing capabilities after damage and establishing sensing pathways in hard-to-reach locations. Application demonstrations in environmental and agricultural monitoring and wearable sensing systems for humans and robots highlight the versatility of this living fungal sensor platform, suggesting promising opportunities in healthcare and the environment.
    Keywords:  biohybrids; biomanufacturing; engineered living materials
    DOI:  https://doi.org/10.1073/pnas.2530456123
  9. Proc Natl Acad Sci U S A. 2026 Jun 23. 123(25): e2605221123
    Collapsible scissored surfaces.
    Noah Toyonaga, Seri Nishimoto, Colter J Decker, Robert J Wood, Tomohiro Tachi, L Mahadevan.
      We introduce an additive approach for the design of a class of transformable structures based on two-bar linkages ("scissor mechanisms") joined at vertices to form a two-dimensional mesh which we call a pantograph lattice. Our approach shows how these lattices unfold from a one-dimensional collapsed state to two-dimensional surfaces of single and double curvature. We provide an algorithm for growing pantograph structures that allows us to explore the full space of possible mechanisms, and we use it to computationally design and physically assemble a series of examples of varying complexity. We finally demonstrate a streamlined method for automated fabrication of pantograph lattices using multimaterial 3D printing.
    Keywords:  geometric metamaterial; linkage; mechanism; origami
    DOI:  https://doi.org/10.1073/pnas.2605221123
  10. Mater Horiz. 2026 Jun 08.
    Bioinspired design of hierarchical structured hydrogels with extraordinary lubrication and load-bearing capacity.
    Xiaoduo Zhao, Xinyuan Kou, Weiyi Zhao, Yibo Chen, Yunsong Kong, Jinshuai Zhang, Zhengfeng Ma, Yunlei Zhang, Bo Yu, Shuanhong Ma.
      Conventional homogeneous hydrogels typically face an inherent trade-off between mechanical strength and lubrication performance. Achieving high load-bearing capacity requires dense crosslinking and tight chain entanglement, which inevitably restrict water uptake and suppress the formation of effective hydration layers. Herein, inspired by the anisotropic architecture of natural ligaments, we developed a robust lubricious hydrogel material (STOC-D) through synergistic spontaneous tensile orientation under confinement (STOC) processing and surface dissociation modification. The STOC process generates highly aligned polymer chains and densely packed microcrystalline domains that serve as robust physical crosslinks, effectively restricting chain slippage and crack propagation. This yields exceptional mechanical properties, including a tensile strength of 54.5 MPa, an elastic modulus of 62.7 MPa, and a tear energy of 25.7 kJ m-2. Subsequent surface dissociation creates a modulus gradient featuring a soft, highly hydrated outer layer rich in dangling chains, which enables rapid water infiltration and the formation of a stable hydration lubrication layer. As a result, the STOC-D hydrogel achieves ultralow coefficients of friction against both metallic and biological surfaces. Furthermore, in vitro cytotoxicity and in vivo subcutaneous implantation studies confirm its excellent biocompatibility. By successfully decoupling bulk mechanical reinforcement from surface hydration, this strategy overcomes the longstanding strength-lubrication trade-off in hydrogels, offering a promising method for load-bearing biomedical applications.
    DOI:  https://doi.org/10.1039/d6mh00765a
  11. ACS Polym Au. 2026 Jun 10. 6(3): 906-917
    Mechanically Enhanced Ultrashort Peptide Hydrogels for pH-Triggered Release.
    Pasqualina Liana Scognamiglio, Carlo Diaferia, Mariantonietta Pizzella, Antonella Accardo, Giancarlo Morelli, Diego Tesauro.
      Ultrashort peptide-based hydrogels represent an attractive class of supramolecular soft materials due to their minimalistic design, chemical versatility, and potential for translational applications. Classical Fmoc-dipeptides, particularly Fmoc-FF, are well established as efficient low-molecular-weight hydrogelators; however, controlling their aqueous solubility and gelation behavior across physiologically relevant conditions remains a key design challenge for injectable and in situ forming materials. Here, we report a pH-responsive injectable hydrogel based on a dipeptide incorporating the unnatural amino acid Fmoc-β-(3-pyridyl)-l-alanine (Fmoc-3-Pal-OH). Introduction of the pyridyl moiety provides a well-defined protonation-deprotonation equilibrium that acts as a molecular switch to regulate the supramolecular self-assembly. Deprotonation in the pH range 6.0-8.0 promotes spontaneous hydrogel formation under mild conditions, while protonation at acidic pH induces a controlled network disassembly. The hydrogel system was comprehensively characterized as a function of the concentration and buffer conditions using fluorescence spectroscopy, circular dichroism, Fourier-transform infrared spectroscopy, scanning electron microscopy, and rheology. pH modulation enables fine control over nanofibrillar organization and viscoelastic properties, yielding mechanically stable hydrogels with tunable stiffness values comparable to those of soft biological tissues. The pH-dependent assembly behavior was further exploited to regulate drug release. Encapsulation of curcumin as a hydrophobic model compound demonstrated high loading capacity and sustained release under neutral conditions, while acidic pH triggered an accelerated release through protonation-induced network collapse. Overall, the results achieved by this research open the way to a simple and robust molecular design strategy to overcome key limitations of conventional Fmoc-based hydrogelators and highlight the potential of protonation-controlled ultrashort peptide assemblies as adaptable polymer-like networks for stimuli-responsive soft materials and drug delivery applications.
    Keywords:  drug delivery; pH-Responsive hydrogels; peptide-based hydrogels; stimuli-responsive materials; supramolecular self-assembly
    DOI:  https://doi.org/10.1021/acspolymersau.6c00020
  12. J Colloid Interface Sci. 2026 Jun 12. pii: S0021-9797(26)01097-0. [Epub ahead of print]723 140920
    Electrical writing of multi-responsive polysaccharide hydrogel enabling integration of programmable deformation and information storage.
    Weiwen Xu, Si Wu, Tao Feng, Qingmiao Wang, Xiaowen Shi.
      Smart hydrogels are capable of sensing and responding to external stimuli, demonstrating promising application in hydrogel actuators, soft robotics and other fields. The integration of hydrogel deformation with information encryption is important to help improve the storage density and security of information. In this study, a simple anodic electrical writing method is employed to graft catechol onto a chitosan/agarose double-network hydrogel, thereby enabling programmable spatial control of the patterned hydrogel. Meanwhile, the grafting process affects the physicochemical properties of the hydrogel, resulting in self-deformation in different solutions. Additionally, the introduction of dynamic boronate ester bonds endows the hydrogel with reversible multiple stimulus responsiveness (e.g., pH, glucose, and temperature), thus achieving reconfigurable deformation behaviors. The synergistic incorporation of electrically written information (Morse code) with the complex deformation of the hydrogel enables dual encryption. Owing to the redox property of catechol, different electrical signals can be generated in the written and unwritten areas. The security of the information is enhanced by using the electrical signals and Morse code for information reading. Furthermore, the hydrogel retains its deformation capability after 10 cycles, and information stored within the written area remains readable via electrical signals even after 30 days. This multi-responsive polysaccharide hydrogel prepared by electrical writing not only provides new insights for natural polysaccharide hydrogel actuators, but also stimulates their application potential in the field of information storage and encryption.
    Keywords:  Chitosan; Complex deformation; Electrical writing; Information storage; Multiple responsiveness
    DOI:  https://doi.org/10.1016/j.jcis.2026.140920
  13. Soft Matter. 2026 Jun 17. 22(23): 4093-4100
    Chemically triggered rapid degradation of tetraPEG gels cross-linked with a diacylhydrazine-containing cross-linker.
    Satsuki Sekiguchi, Takamasa Sakai, Kousuke Tsuchiya.
      Controlling the degradability of cross-linked polymer materials is essential for designing soft materials that combine structural stability during use with on-demand disassembly at the desired time. Herein, we report a chemically degradable tetra-armed poly(ethylene glycol) (tetraPEG) hydrogel cross-linked with a newly designed diacylhydrazine-containing cross-linker. The cross-linker incorporates cysteine residues as reactive sites and a diacylhydrazine moiety as a chemically cleavable unit that undergoes rapid scission in response to sodium hypochlorite (NaClO). The cross-linker exhibited efficient reactivity toward maleimide compounds through thiol-maleimide click chemistry, enabling the formation of a stable tetraPEG network from tetraPEG bearing maleimide end groups. Upon treatment with NaClO, the tetraPEG gel underwent rapid degradation in a concentration-dependent manner. Microscopic analysis further revealed that the squared diameter decreased nearly linearly with time, consistent with a diffusion-limited surface erosion process. The degraded polymer component was almost identical to the original tetraPEG precursor, indicating that network cleavage occurred selectively at the diacylhydrazine units to release soluble tetraPEG chains. These results demonstrate that diacylhydrazine-based cross-linking provides an effective strategy for constructing robust yet chemically degradable hydrogel networks with controllable degradation behavior.
    DOI:  https://doi.org/10.1039/d6sm00301j
  14. ACS Appl Mater Interfaces. 2026 Jun 19.
    Bio-Inspired Topologically Constrained, Interlocking-like Cellulose Architectures via Sacrificial Oligomer Templating.
    Yipeng Chen, Kayoko Kobayashi, Qingfeng Sun, Masahisa Wada.
      Overcoming the inherent strength-toughness trade-off remains a persistent challenge for bioinspired structural materials. Here we develop a high-performance topologically interlocking-like cellulose (TICell) via sacrificial oligomer templating followed by post-cross-linking. Calcium phosphate oligomeric clusters (CPOs) are introduced as transient inorganic templates to confine space within a regenerated cellulose network. Subsequent citric-acid treatment removes the templates while simultaneously covalently cross-linking cellulose, effectively "locking in" a topologically constrained architecture after demineralization. Multiscale characterization shows that the cellulose crystalline framework is largely retained, yet the nanoscale organization reorganizes qualitatively into a continuous, percolated network composed of puzzle-like interlocking modules. This interlocked topology reshapes damage evolution: catastrophic crack run-away is suppressed and energy is dissipated progressively through crack deflection and stepwise advance. As a result, TICell exhibits a strength of 226 MPa and a fracture toughness of 7.0 kJ m-2, representing several-fold improvements over biological materials and conventional polymers. These findings suggest a sustainable route to damage-tolerant, biobased structural materials in which mechanical performance is governed primarily by topology, rather than by crystallinity or composition alone.
    Keywords:  bioinspired; cellulose; inorganic oligomer; mechanical properties; topological structure
    DOI:  https://doi.org/10.1021/acsami.6c05062
  15. Chem Soc Rev. 2026 Jun 12.
    Engineering coordination bonds for bioinspired responsive polymers.
    Muqing Si, Weihao Feng, Tao Chen, Wei Lu.
      Responsive polymeric materials capable of converting weak and heterogeneous environmental cues into adaptive macroscopic functions are essential for emerging technologies spanning soft robotics, sensing, biointerfaces, and autonomous systems. Coordination-crosslinked polymer networks (CCPNs), constructed by embedding dynamic metal-ligand interactions into polymer matrices, have emerged as a powerful materials platform for this purpose, owing to the unique tunability, reversibility, and multifunctionality of coordination bonds. Unlike conventional covalent or other supramolecular crosslinks, coordination bonds provide continuously adjustable bond strength, well-defined geometry, stimulus-sensitive equilibria, and access to electronic, redox, and catalytic transitions, enabling direct transduction of physical and chemical stimuli into mechanical, optical, and morphological responses. Despite rapid progress, a unified understanding that links coordination chemistry at the molecular level to material responsiveness across length and time scales remains lacking. In this review, we systematically examine how the intrinsic properties of coordination bonds give rise to material responsiveness in CCPNs. We first introduce fundamental coordination chemistry concepts relevant to responsive network design and discuss how these factors govern bond dynamicity, exchange kinetics, and stimulus sensitivity within polymer networks. We then analyse how coordination dynamics manifest as macroscopic responses, with a focus on stiffness variation, optical and chromic switching, shape memory and actuation, and life-like homeostatic behaviors driven by non-equilibrium bond cycling. Moving beyond single-interaction systems, we highlight recent advances in bond coupling strategies, where multiple coordination motifs or coordination bonds integrated with other supramolecular bonds, dynamic covalent bonds, or mechanical bonds generate hierarchical relaxation, orthogonal responsiveness, and synergistic function expression reminiscent of biological materials. Finally, we discuss key challenges and outline future opportunities for transforming coordination chemistry from a crosslinking motif into a molecular-level control framework for engineering responsive and life-like soft materials.
    DOI:  https://doi.org/10.1039/d5cs01074h
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