Highly Programmable Liquid Crystalline Polyurethane/MXene Hybrids for Large‐Strain, High‐Work‐Capacity Artificial Muscles

ABSTRACT Liquid crystal elastomers (LCEs) are attractive for soft actuators and biomimetic systems owing to their rapid responsiveness and reversible deformations, yet achieving simultaneous high actuation stress and strain for complex macroscopic motions remains challenging. Herein, we report a liquid‐crystalline polyurethane (LCPU)/MXene hybrid network, fabricated via in situ polymerization, that overcomes this long‐standing trade‐off. The flexible polydimethylsiloxane (PDMS) imparts large reversible deformability, while covalently anchored MXene simultaneously reinforce mechanical strength and enable efficient photothermal conversion, yielding robust thermal‐ and light‐driven actuation. The dynamic hydrogen bonding network confers on‐demand network reconfigurability and shape programmability within an optimal temperature window. The resulting actuators achieve a thermal‐driven stress of 0.91 MPa at 88% strain, while it increased to 1.58 MPa under near‐infrared (NIR) stimulation, yielding an exceptionally high work capacity of 546 kJ m ^{− 3} . An active‐passive composite actuator constructed from LCPU/MXene demonstrates programmable morphing under thermal stimuli. When employed as artificial biceps and quadriceps of robotic counterparts, these actuators perform diverse large‐amplitude actuation tasks such as lifting and pushing under remote near‐infrared irradiation. This thermal and light‐driven LCPU/MXene system holds considerable promise as a versatile platform for artificial muscles, adaptive aerospace actuators, and related intelligent applications.