“…Various photomechanical materials, such as polymers, elastomers, liquid‐crystalline materials, and molecular crystals, have been reported, to date. In particular, photomechanical crystals have attracted increasing attention because they not only have great potential for applications in light harvesting, mechanical actuators, molecular machines, optical sensors, and smart switches, but also provide the opportunity to understand their performance through XRD methods by solving ordered molecular structures . Compared with polymers, elastomers, and liquid‐crystalline materials, molecular crystals possess many advantages, such as faster response times, shorter recovery times, a higher Young's modulus, and a well‐defined crystal structure .…”