LAUSR

In contrast to most synthetic hydrogels, biological gels are made of fibrous networks. This architecture gives rise to unique properties, like low concentration, high porosity gels with a high mechanical responsiveness as a result of strain-stiffening. Here, we used a synthetic polymer model system, based on polyisocyanides, that we crosslinked selectively inside the bundles. This approach allows us to lock in the fibrous network present at the crosslinking conditions. At minimum crosslink densities, we are able to freeze in the architecture, as well as the associated mechanical properties. Rheology and X-ray scattering experiments show that we able to accurately tailor network mechanics, not by changing the gel composition or architecture, but rather by tuning its (thermal) history. Selective crosslinking is a crucial step in making biomimetic networks with a controlled architecture.Unlike synthetic hydrogels, biological gels are made of fibrous networks which give rise to unique properties, such as high porosity and mechanical responsiveness. Here the authors use polyisocyanide-based gels and selectively crosslink inside the bundles to lock the fibrous network and thus control the architecture and the mechanics.