Combining Mechanical Tuneability with Function: Biomimetic Fibrous Hydrogels with Nanoparticle Crosslinkers

Fibrous networks of biopolymers possess unique properties: mechanical stability at low concentrations, an extremely porous architecture, and strong stiffening at small deformations. An outstanding challenge is to find methods that allow to tailor the mechanical properties of these bionetworks or their synthetic equivalents without changing the polymer concentration, which simultaneously changes all other hydrogel properties. Here, networks of dilute (0.1 wt.%) fibrous hydrogels are prepared and crosslink them with functional rod-shaped nanoparticles. The crosslinking is observed to induce an architectural change that strongly affects the mechanical properties of the hydrogels with a 40-fold increase in stiffness. The effect is strongest at the lowest polymer and particle concentrations (99.8% water) and is tailorable through tuning the crosslink density. Moreover, the nanoparticle components in the composite offer the opportunity to introduce additional functions; gels with magnetic and conductive properties are reported. However, through the generic crosslinking approach of a fibrous network with decorated nanoparticle crosslinkers as presented in this work, virtually any functionality may be introduced in highly responsive hydrogels, providing a guide to design next generations of multi-functional soft materials.