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Bridging crystallinity and softness: dynamic coordination and functional integration in MOF–hydrogel hybrid materials
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DOI：10.1016/j.pmatsci.2026.101784.png)
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Abstract
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Metal–organic framework (MOF)–hydrogel systems have emerged as a highly versatile class of hybrid soft materials, yet the field remains conceptually fragmented. While current literature is largely organized around isolated formulations, fabrication routes, and phenomenological applications, it places comparatively limited emphasis on the unifying principles that connect crystalline structure, interfacial chemistry, network dynamics, mass transport, and functional outcomes across scales. To shatter this conceptual limitation, this Review decisively recasts MOF–hydrogel systems not as static filler-containing composites or passive delivery matrices, but as programmable spatiotemporal microenvironment processors. We define the intrinsic limitations of standalone constituents, and then establish the fundamental design logic by which their integration yields deeply coupled hard–soft systems. Moving beyond simple physical blending, we elucidate how interfacial chemistry transforms nominal phase boundaries into active functional interphases that dynamically regulate force transmission, catalytic accessibility, transport selectivity, and biological recognition. On this basis, we unify viscoelastic programming, mechanical cascades, confined reactive microenvironments, and intrinsic biological modules into a common framework that explains scenario-adaptive function across chronic wounds, oral and craniofacial tissues, and load-bearing osteochondral defects, while also extending beyond regenerative medicine to flexible biointerfaces, bacterial diagnostics, environmental remediation, and responsive closed-loop systems. Importantly, we also examine the translational constraints that continue to limit the field, including incomplete structure–property–function mapping, inconsistent dynamic mechanical testing, ambiguous loading and release metrics, uncertain long-term biosafety, and the practical challenges of scale-up, sterilization, storage, and regulatory alignment. Finally, we outline a future direction in which mechanism-informed inverse design, AI-assisted data integration, hierarchical living-integrated constructs, adaptive biointerfaces, and the deep convergence of chemistry, rheology, immunology, and biofabrication drive the emergence of predictive, spatially structured, and increasingly autonomous microenvironmental materials.
Keywords:
Metal–organic frameworks
Dynamic hydrogels
Functional interphases
Viscoelastic programming
Translational materials design
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