Shape‐Programmable Liquid‐Crystalline Polyurethane‐Based Multimode Actuators Triggered by Light‐Driven Molecular Motors

Abstract In recent years, light‐driven soft actuators have been rapidly developed as enablers in the fabrication of artificial robots and biomimetic devices. However, it remains challenging to amplify molecular isomerization to multiple modes of macroscopic actuation with large amplitude and complex motions. Here, a strategy is reported to build a light‐responsive liquid‐crystalline polyurethane elastomer by phototriggered overcrowded alkene‐based molecular motors. A trifunctional molecular motor modified with an ethylene glycol spacer on the rotor and stator functions as a crosslinker and unidirectional stirrer that amplifies molecular motion into macroscopic movement. The shape‐programmable polymeric film presents superior mechanical properties and characteristic shape‐memory effect. Furthermore, diverse modes of motions including bending, unwinding, and contracting with tunable actuation speed over a wide range are achieved. Such research is hoped to pave a new way for the design of advanced light‐responsive soft actuators and robots.