Skeletal‐Muscle‐Inspired Superstrong Dynamic Covalent Liquid‐Crystal Elastomers With Exceptional Actuation Performance

ABSTRACT As an emerging actuator material for artificial muscles and soft robotics, dynamic covalent liquid‐crystal elastomers (DCv‐LCEs) enable network reorganization through dynamic bond exchange, allowing actuator reprogramming, actuation‐mode tuning, and material recycling. Despite these distinctive advantages, existing DCv‐LCEs still suffer from limited actuation performance for practical applications. Inspired by the critical role of noncovalent interactions in natural skeletal‐muscle actuation, we develop a superstrong DCv‐LCE (SS‐DCv‐LCE) by deliberately engineering a dynamic covalent liquid‐crystal network that simultaneously incorporates hydrogen‐bonding and metal‐coordination crosslinks. The dual noncovalent crosslinks synergistically reinforce SS‐DCv‐LCE, giving rise to a remarkably high Young's modulus (∼27.6 MPa) and a superhigh strength (∼30.7 MPa) at room temperature, while also imparting significantly enhanced mechanical robustness at elevated temperatures. As a result, SS‐DCv‐LCE delivers an actuation stress of up to 1.6 MPa and a work capacity of up to 486.1 kJ m −3 , which are ∼4.5‐ and ∼12.1‐fold higher than those of human skeletal muscle, respectively, and also far exceed those of existing state‐of‐the‐art elastomeric DCv‐LCEs. Moreover, SS‐DCv‐LCE exhibits reprogrammability and reprocessability, enabling reshaping and recycling into actuators with diverse geometries and actuation modes. This work establishes a new network‐architecture design for high‐actuation‐performance DCv‐LCEs, opening opportunities for practical applications in artificial muscles and soft robotics.