MOF‐Induced Pore Confinement: A Strategy for Thermomechanically Robust and High‐Strength Liquid Crystal Elastomers

ABSTRACT Liquid crystal elastomers (LCEs) are premier candidates for soft robotics due to their large, reversible actuation. However, their utility is often restricted by a fundamental trade‐off: as temperature increases, orientational order diminishes, causing a sharp loss in load‐bearing capacity and actuation stress above the isotropic transition. Here, we report a sequential integration strategy that overcomes this thermal limitation by embedding ultrathin Cu‐TCPP metal‐organic framework (MOF) nanosheets within the LCE network. This approach establishes a pore‐confinement‐enabled architecture that restricts segmental relaxation and preserves molecular alignment even under harsh thermal conditions. The resulting LCE‐MOF composites exhibit exceptional mechanical robustness, achieving a tensile strength of 79 MPa at 25°C and maintaining 4.2 MPa at 200°C. Notably, the materials deliver a high actuation stress of 3.9 MPa at 200°C, significantly outperforming composites fabricated via conventional direct mixing. This confinement strategy effectively decouples mechanical integrity from thermal transitions, as demonstrated by a high‐performance passive thermal valve capable of reliable switching in extreme environments. Our work provides a versatile methodology for designing resilient, high‐output soft actuators for aerospace, industrial, and high‐temperature hazardous applications where thermal stability and reliable actuation are critically demanded.