which have attracted considerable research attention. Spiropyran can change from its closed form to the merocyanine (MC) structure under ultraviolet (UV) light, and recover its original form by visible light or heat treatment. [7] Other external stimuli, such as acids or bases, [8] metal ions, and redox potentials [7a,c] can also achieve this reversible isomerization. Unfortunately, most of these stimulus-induced conversions can only occur in solution or soft materials and are hampered in the solid state. As a result, one of the main tasks in the development of solid-state photoresponsive materials for practical applications is achieving an effective stimulus-induced conversion in the solid state. The reason for the limited cisâtrans isomerization in the solid state is the lack of intrinsic structural flexibility, which is required to release stress and strain during the stimulus-induced transformation. The main problem lies in the photo-switching of SP compounds, because of their strong molecular packing in the aggregated state. Such close molecular packing mainly hinders the cisâtrans isomerization, which occurs during photochemical reactions between the SP and MC isomers. Hence, an effective way to solve the current challenges in solid-state photoswitching is to create large free volumes during the isomerization. There are two common methods to achieve this goal. One involves the copolymerization of spiropyran with polymer monomers. [9] For example, Li et al. fabricated a reversible photochromic nanofiber membrane by copolymerizing spiropyran with octadecyl acrylate and blending it with polyvinyl alcohol (PVA)/polyethylenimine (PEI). [9a] However, polymerization is relatively complex and involves rather harsh reaction conditions. Another approach involves the modification of spiropyran with large steric organic molecules. In a previous study, the main goal was to introduce long flexible chains in spiropyran, to increase the free volume. [10] However, long chains always led to a decrease in the thermal stability, and the photochromic properties did not show an obvious enhancement. Currently, researchers are mainly focusing on introducing rigid steric hindrance groups to improve the photochromic properties and the thermal stability. [11] The Xu and Yin's groups reported that the solid-state photochromism of spiropyran was improved by introducing aggregation-induced emission (AIE) molecules, owing to their highly twisted structures, which induced loose packing and provided a larger free volume in the aggregated state. [12] In addition, the Yin group reported that the introduction of naphthalimide provided sufficient free Solid-state materials with reversible properties are highly attractive, owing to versatile applications in security, sensors, bioimaging, and information storage. Unfortunately, obtaining these materials in the solid state remains a huge challenge. Efficient isomerization usually requires sufficient conformational freedom and cannot be achieved without solvents or matrices. In this study, four st...