Host‐Fueled Transient Supramolecular Hydrogels

Abstract Inspired by the dissipative assembly in biological systems, transient hydrogels based on supramolecular interactions have been developed that are under thermodynamic nonequilibrium states. Host–guest interactions possess excellent properties including high selectivity and adjustable association constants, which are beneficial for controlling the properties and behaviors of transient colloidal materials. In this work, a host‐fueled transient supramolecular hydrogel system is reported. The hydrogels based on host–guest interactions are formed by addition of a chemical fuel, α‐cyclodextrin (α‐CD), to the aqueous solutions containing Pluronic F127 and α‐amylase. Meanwhile, as the host molecule of α‐CD consumes, the hydrogel networks start to collapse. The lifetime of the transient supramolecular hydrogels can be precisely controlled by adjusting the temperature and hydrogel composition, and repeated sol‐to‐gel‐to‐sol transitions can be realized by refueling the system with α‐CD. This study provides a new approach to regulate the nonequilibrium host–guest inclusion system by fueling it with host molecules.