The integration of advanced functions and diverse practical applications calls for multifunctional liquid crystal elastomers (LCEs); however, the structure-intrinsic luminescence and excellent mechanical properties of LCEs have not yet been explored. In this study, clusteroluminescence (CL)-based LCEs (CL-LCEs) are successfully fabricated without depending on large conjugated structures, thereby avoiding redundant organic synthesis and aggregation-caused quenching. The experimental and theoretical results reveal that secondary amine (–NH–) and imine (–C = N–) groups play vital roles in determining the presence of fluorescence in CL-LCEs. Based on the above observation, the strategy universalization and a molecular library for constructing CL-LCEs are further demonstrated. Meanwhile, the dynamic bond of imine bonds endows the CL-LCE system with rapid self-healing under mild conditions (70 °C in 10 min), excellent stretchability, and adaptive programmable characteristics. Furthermore, the self-luminescent performance enables visual detection of the self-healing process. Finally, CL-based information storage and anticounterfeiting are successfully realized and their applications in fiber actuators and fluorescent textiles are demonstrated. The distinctive luminescence and dynamic chemistry presented in this work has significant implications in elucidating the mechanism of CL and providing new strategies for the rational design of novel multifunctional LCE materials.