ABSTRACTLiquid crystal elastomers (LCEs) are liquid crystal polymers with moderate crosslinking that exhibit elasticity in both their isotropic and liquid crystal states. These materials can be programmed through chemical design and geometric configuration to achieve autonomous actuation at specific temperatures. Typically, the autonomous actuation temperature of LCEs exceeds the phase transition temperature of their isotropic states, with most reported LCEs requiring temperatures above 100°C. Such high temperatures pose challenges for use in soft robotics due to increased energy consumption and limited operational flexibility. In this study, we introduce a small amount of polycaprolactone (PCL) into the main chain of LCEs, effectively lowering their phase transition temperature while maintaining over 90% of the reversible shrinkage strain characteristic of pure LCEs. By adjusting the PCL content, the number of twists, and the helix density, we successfully obtained an LCE‐PCL actuator with improved autonomous actuation performance at temperatures ranging from 45°C to 105°C. Moreover, by modulating the degree of torsion and the operating temperature, the LCE‐PCL autonomous actuator demonstrates the ability to perform complex motions, such as reversing and parking. This work offers new insights into the design and application of LCEs with reduced phase transition temperatures and enhanced self‐driving capabilities.
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