Solvent‐Assisted Preparation of Recyclable Multidimensional Fluorescent Actuators

Light‐responsive elastic crystals and polymers are widely used in the fabrication of smart actuators. However, crystal morphology, which is strongly dependent on the molecular self‐assembly, remains difficult to control, while the performance of polymers is significantly affected by their components, limiting their practical applications. To balance the advantages of crystal‐ and polymer‐based materials, in this study, solvent molecules were doped into small‐molecule photosensitive materials ( E ‐ BI ‐ TPA ‐ CS ) to weaken the intermolecular interactions and enable the precise, facile, and fast preparation of flexible multidimensional photoactuators through simple artificial manipulations such as stretching. The as‐prepared actuator combines the high energy density of crystalline materials with the tailorable properties of polymers. Upon UV or visible light irradiation, E ‐ BI ‐ TPA ‐ CS undergoes E ‐ Z isomerization, driving actuator deformation. The reversible isomerization and simple fabrication process make the actuators recyclable. Additionally, these photoresponsive materials can adhere to metal surfaces to facilitate the construction of photoswitches without complex operations, such as metal deposition. Furthermore, the introduction of the aggregation‐induced emission (AIE) unit enables visual tracking of the actuation process. This resin‐like material offers a new perspective on multifunctional materials by effectively bridging the gap between crystalline and polymeric systems, optimizing the preparation of actuators, and improving their performance.