Thermal reprogrammability is essential for new‐generation large dry soft actuators, but the realization sacrifices the favored actuation performance. The contradiction between thermal reprogrammability and stability hampers efforts to design high‐performance soft actuators to be robust and thermally adaptable. Now, a strategy has been developed that relies on repeatedly switching on/off thermal reprogrammability in liquid‐crystalline elastomer (LCE) actuators to resolve this problem. By post‐synthesis swelling, a latent siloxane exchange reaction can be induced in the common siloxane LCEs (switching on), enabling reprogramming into on‐demand 3D‐shaped actuators; by switching off the dynamic network by heating, actuation stability is guaranteed even at high temperature (180 °C). Using partially black‐ink‐patterned LCEs, selectively switching off reprogrammability allows integration of completely different actuation modes in one monolithic actuator for more delicate and elaborate tasks.

Stimuli-responsive materials offer a distinguished platform to build tether-free compact soft robots, which can combine sensing and actuation without a linked power supply. In the past, tubular soft robots have to be made by multiple components with various internal channels or complex cavities assembled together. Moreover, robust processing, complex locomotion, simple structure, and easy recyclability represent major challenges in this area. Here, it is shown that those challenges can be tackled by liquid crystalline elastomers with allyl sulfide functional groups. The light-controlled exchange reaction between allyl sulfide groups allows flexible processing of tubular soft robots/actuators, which does not need any assisting materials. Complex locomotion demonstrated here includes reversible simultaneous bending and elongation; reversible diameter expansion; and omnidirectional bending via remote infrared light control. Different modes of actuation can be programmed into the same tube without the routine assembly of multiple tubes as used in the past. In addition, the exchange reaction also makes it possible to use the same single tube repeatedly to perform different functions by erasing and reprogramming.

Achieving 3D structures that can be reversibly formed from dry 2D polymer films is useful for the development of suitable smart materials capable of converting an external stimulus into a mechanical response.

A vitrimer-based LCE actuator subtly mitigates the conflict between processability and actuation durability by reducing the catalyst content.

Liquid-crystalline elastomers (LCEs) are excellent soft actuator materials for a wide range of applications, especially the blooming area of soft robotics. For entirely soft LCE robots to exhibit high dexterity and complicated performance, several components are typically required to be integrated together in one single robot body. Here, we show that seamless multicomponent/multimaterial three-dimensional (3D) LCE robots can be created via simultaneously welding and aligning LCE materials with different chemical compositions and physical properties without other additives such as tapes and glues (just like metal welding). Both welding and aligning of the LCE materials rely on thermal polymerization of preformed LCE films with reactive acrylate groups. This method provides an easy way to robustly fabricate arbitrary 3D desirable geometries with strongly stable reversible actuations and multifunctionalities, which greatly enlarges and benefits the future applications and manufacturing of LCE soft robots.