Photoresponsive supramolecular materials have been fabricated by controlling the density of reversible cross-links or the distribution of movable cross-links. This study prepared photoresponsive polyurethane (CD-Azo-PU) based on controlling the crystallization of the hard segments in polyurethane (PU) by complexation between azobenzene (Azo) and cyclodextrins (CDs). CD-Azo-PU incorporated polyurethane as the main chain and a 1:2 inclusion complex between Azo and γCD as a movable crosslink point. Upon ultraviolet light (UV, λ = 365 nm) irradiation, the photoresponsiveness of CD-Azo-PU bent toward the light source (defined as positive), while that of the linear Azo polyurethane (Azo-LPU) without TAcγCD-diOH as a movable crosslinker bent in the direction opposite the light source. The bending rates were determined to be 0.058°/s for CD-Azo-PU and 0.027°/s for Azo-LPU, indicating that the bending rate for CD-Azo-PU was faster than that for Azo-LPU. By incorporating movable cross-links into CD-Azo-PU, we successfully achieved specific photoresponsive actuation with an enhanced rate.