Robust Mechanically Interlocked Network Ionogels

Abstract Ionogels have attracted considerable attention as versatile materials due to their unique ionic conductivity and thermal stability. However, relatively weak mechanical performance of many existing ionogels has hindered their broader application. Herein, we develop robust, tough, and impact‐resistant mechanically interlocked network ionogels ( IG MINs) by incorporating ion liquids with mechanical bonds that can dissipate energy while maintain structural stability. Profiting from the dynamic yet stable nature of the mechanically interlocked networks, IG MINs exhibit high tensile strength (9.6 MPa), fracture energy (39 kJ/m 2 ), and toughness (25.9 MJ/m 3 ), along with a high elongation rate (473 %) and excellent impact resistance and shape memory, resulting in overall performance that surpasses most reported ionogels. Furthermore, in the application of strain sensors for monitoring the gait of crawling robots, the toughness and robustness of IG MINs ensure their ability to consistently output stable electrical signals during the stretching and contraction processes, thereby highlighting their practical application potential. Our work provides a new research strategy for toughening ionogels and promotes the development of mechanically interlocked materials.