Towards tissue‐like material properties: inducing in situ adaptive behavior in fibrous hydrogels

The material's properties of biological tissues are unique. Nature is able to spatially and temporally manipulate (mechanical) properties while maintaining responsiveness towards 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 polyisocyanides (PIC), that is noncovalently linked to a responsive crosslinker. The introduction of the crosslinker 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 materials design is crosslinking at the fibrillar level using nanoparticles, which, simultaneously may be used to introduce more advanced properties. This article is protected by copyright. All rights reserved.