Here, we present single crystalline capsules of a photoresponsive molecule produced by simple recrystallization from organic solutions without direct human processing. During the crystal growth process, a movie was taken of the capsule taking in the organic solution. The capsules responded rapidly (<1 s) to the UV light stimuli and released the captured solution or solute. In principle, they can take in any substance dissolved in organic solvents, and their size can be controlled. Moreover, the capsule can be broken by multi-photon excitation using a near-infrared laser within the biological window. Furthermore, because the molecular packing in the crystal is unidirectional, the response can be controlled by the polarization of the light. This study shows the new potential of photoresponsive molecules.