Dynamic Liquid Crystal Elastomers for Body Heat‐ and Sunlight‐Driven Self‐Sustaining Motion via Material‐Structure Synergy

Self‐sustained actuators powered by natural, low‐energy sources based on liquid crystal elastomers (LCEs) are attractive as they offer high safety, abundant energy availability, and practicality in applications. However, achieving stable self‐sustaining motion with low‐energy sources requires high actuation strain rates within a narrow temperature range near ambient conditions—a great challenge as LCEs with low nematic‐to‐isotropic transition temperatures (Tni) generally exhibit reduced actuation strain and strain rates. To address this, we synthesized a carbon nanotube‐doped LCE with a low Tni and reversible Diels‐Alder crosslinks, termed DALCE, and readily (re)fabricated it into specific structures (e.g., twisted‐and‐coiled or bimorph shapes). By leveraging material‐structure synergy, we achieved both low Tni and high actuation strain rates, enabling self‐rolling, self‐breathing and autonomous twisting‐untwisting movements powered by ambient/body temperature or natural sunlight. This low‐energy, self‐sustained actuator design opens new possibilities for LCE‐based biomedical applications and naturally powered automatic devices.