Toward Recyclable Liquid Crystal Elastomers Enabled by Imine–Boroxine Dual Dynamic Covalent Bonds for Multi‐Form Sustainable Applications

ABSTRACT Amid growing concerns over plastic pollution and the pressing need for sustainable materials, achieving closed‐loop recycling of liquid crystal elastomers (LCEs) with permanent cross‐links remains a significant challenge. Here, we report a fully recyclable LCE system featuring a dual dynamic covalent network constructed from boroxine and imine bonds. The synergistic effect between these dynamic linkages enables efficient network rearrangement under mild conditions, allowing shape programming at 40°C within 10 min and reprocessing at 40°C in 1 h. Notably, the reversible dissociation of boroxine bonds facilitates depolymerization of the cross‐linked network into soluble oligomers at room temperature, enabling cyclic reprocessing into diverse functional forms such as bilayer actuators, fibers, and patterns, thereby lowering the technical barriers to multiform fabrication. In addition, the clusteroluminescence (CL) from imine and secondary amine units allows fluorescence visualization under UV light across various morphologies, enabling precise material identification during recycling. This work provides a versatile and sustainable platform for the closed‐loop manufacturing of smart LCE materials.