Toward Tissue-Like Material Properties: Inducing In Situ Adaptive Behavior in Fibrous Hydrogels

The materials properties of biological tissues are unique. Nature is able to spatially and temporally manipulate (mechanical) properties while maintaining responsiveness toward a variety of cues; all without majorly changing the material's composition. Artificial mimics, synthetic or biomaterial-based are far less advanced and poorly reproduce the natural cell microenvironment. A viable strategy to generate materials with advanced properties combines different materials into nanocomposites. This work describes nanocomposites of a synthetic fibrous hydrogel, based on polyisocyanide (PIC), that is noncovalently linked to a responsive cross-linker. The introduction of the cross-linker transforms the PIC gel from a static fibrous extracellular matrix mimic to a highly dynamic material that maintains biocompatibility, as demonstrated by in situ modification of the (non)linear mechanical properties and efficient self-healing properties. Key in the material design is cross-linking at the fibrillar level using nanoparticles, which, simultaneously may be used to introduce more advanced properties.