Photoresponsive crystalline systems mimicking bio-functions are prepared using photochromic diarylethenes. Upon UV irradiation of the diarylethene crystal, the photogenerated closed-ring isomers self-aggregate to form needle-shaped crystals on the surface. The rough surface shows the superhydrophobic lotus effect. In addition, the rose-petal effects of wetting, the anti-reflective moth-eye effect, and a double-roughness structure mimicking the surface of a lotus leaf are observed by controlling the heating procedures, UV irradiation processes, and molecular structural modification. By changing the molecular structure, a superhydrophilic surface mimicking a snail shell can be generated. We also find the crystal of a diarylethene derivative that shows a photosalient effect. The effect is observed partly due to the hollow structure of the crystal. It is demonstrated that a photo-response similar to the response of impatiens plant to stimulation is observed by packing small beads in the hollow. These photoresponsive functions are unique, and they demonstrate a macroscopic response by means of microscopic molecular movement induced by light. In the future, such a molecular assembly system will be a promising candidate for fabricating photoresponsive architectures and soft robots.