Intrinsically Photothermal‐Driven and Reconfigurable Liquid Crystal Elastomer Actuators Enabled by Multifunctional Dynamic Covalent Organic Photothermal Molecules

Abstract Intrinsically photothermal‐responsive soft actuators possessing reconfigurability have attracted great attention due to their ability to change their actuation mode to satisfy diverse practical applications. However, challenges remain in designing and fabricating organic photothermal molecules featuring polymerizable or cross‐linkable groups, especially those with multifunctional properties. Here, a novel class of versatile light‐driven reconfigurable liquid crystal elastomer (LCE) materials, denoted as PUOLCE, has been developed. The multifunctional dynamic covalent organic photothermal molecules, serving as chain extenders, photothermal agents, and dynamic covalent bond precursors, are chemically bonded into LCEs, thereby endowing the LCEs with photothermal‐responsiveness and dynamic properties. The intrinsic photothermal effect of PUOLCE allows the exchange reaction of dynamic oxime‐carbamate bonds to undergo rapid welding under near‐infrared (NIR) light. Leveraging the NIR‐assisted welding strategy, the PUOLCE‐based building units are capable of assembling into various complex actuators with new deformation modes. Besides, the assembled actuators can be easily reconfigured to perform different mechanical tasks (e.g., flower blooming, grasping objects, and elevating objects) under NIR illumination. Furthermore, the PUOLCE actuators can be controlled globally or locally for light‐driven locomotion by controlling the area exposed to the NIR irradiation. This work provides insights into the development of adaptive soft actuators with tunable shape‐morphing capabilities.