Summary: Light‐induced reversible changes in elasticity of semi‐interpenetrating network (semi‐IPN) films bearing azobenzene moieties were achieved under both ultraviolet (UV) and visible light irradiation. The semi‐IPN film was prepared by a cationic copolymerization of azobenzene‐containing vinyl ethers in a linear polycarbonate (PC) film as a matrix. When the irradiation was switched on and off, the semi‐IPN film showed rapid reversible deformation with the same behavior occurring over a range of wavelengths, including both the UV and visible regions. The observed reversible deformation of the film was attributed to the decrease in the film's elasticity, which was assumed to be caused by the frequent trans‐cis cycling isomerization of azobenzene moieties taking place during the UV and visible light irradiation. This cycling makes it difficult for the azobenzene groups to aggregate, thus hindering their ability to function as pseudo‐crosslinking points.
