Programmable Soft Actuator with Multi‐Responsiveness Based on Conductive MOF‐Liquid Crystal Polymer Composite

ABSTRACT Independent dual alignment of the anisotropic, conductive metal–organic framework (MOF) crystals and liquid‐crystal polymer (LCP) network enables a multi‐responsive soft actuator capable of both UV‐driven photothermal and electrothermal operation. In this design, LC alignment ensures reversible actuation, whereas Cu 3 (HHTP) 2 (HHTP = 2,3,6,7,10,11‐hexahydroxytriphenylene) alignment governs bilayer structure and charge transport pathways, enabling advanced functionalities including on/off switching, region‐selective actuation, and programmable directionality. In the photothermally driven mode, strong UV absorption and efficient non‐radiative relaxation of Cu 3 (HHTP) 2 , combined with a horizontal bilayer structure, induce rapid and reversible bending. A Hercules beetle‐inspired horn actuator lifted loads up to 40 times its own weight. In the electrically driven mode, Cu 3 (HHTP) 2 produced uniform Joule heating and large bending only when horizontally aligned, reflecting the creation of long‐range conductive pathways. As a proof of concept, this principle was applied to a self‐protective smart wire that autonomously disconnects under overcurrent. Collectively, these findings provide valuable insights into the alignment, manipulation, and utilization of anisotropic conductive MOFs for diverse applications, including soft grippers, adhesive/reconfigurable electrical wiring, and microelectronics.