The need for materials capable of exhibiting different properties upon exposure to an external stimulus has led to many developments, notably in the field of supramolecular chemistry. Indeed, weak hydrogen-bonding interactions have enabled the preparation of materials with switchable properties, such as in the case of polymers reinforced with cellulose nanocrystals that, triggered by the presence of water, exhibit a dramatic change of the materials’ mechanical properties. This project intends to develop stimuli-responsive materials based on biocompatible polymers that form networks whereby localized interactions and hydrophilicity are tuned by adjusting the copolymer composition. The storage moduli of the studied materials are in the GPa range; upon triggering the modulus drastically decreases (MPa range).