Supramolecular Gel‐to‐Gel Transition Induced by Nanoscale Structural Perturbation via the Rotary Motion of Feringa's Motor

Abstract Supramolecular rather than covalent molecular engineering on Feringa motors can provide an alternative toolkit for tuning the properties of motorized materials through appropriate supramolecular structural perturbations, which are underexplored. Herein, a multicomponent supramolecular gel system is successfully prepared by employing an ultra‐low molecular weight gelator and a modulator‐Feringa motor. The electron microscopic, spectroscopic, and rheological data revealed that the morphology and mechanical properties of the gel can be tuned via a crystallographic mismatch branching (CMB) mechanism simply by adding varied amounts of motor modulators. Notably, the rotary motion of the motor is preserved in such a multicomponent gel system, and the morphology and rheology of the gel can be further altered by the motor's rotary motion that promotes the structural perturbation, resulting in seldomly seen gel‐to‐gel transition events. The work shown here offers prospects to utilize a supramolecular perturbation strategy to deliver responsiveness from molecular motors to the corresponding bulk materials.