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Structural color materials with reversible stimuli‐responsiveness to external environment have been widely used in sensors, encryption, display, and other fields. Compared with other stimuli, visible light is highly controllable both temporally and spatially with less damage to materials, which is more suitable for structural color patterning. Herein, a new diselenide‐containing shape memory material is prepared and used for creating patterns via visible light stimulus. In this system, the structural color originates from birefringence of stretched materials, whose shapes can be fixed while maintaining the mechanical stress. The fixed stress can be released by diselenide metathesis under visible light irradiation. By regulating the wavelength or irradiation time with a commercial projector, the pattern with tunable structural colors is realized and the structural color pattern can be erased and rewritten arbitrarily. During the patterning process, the optical signal is first stored as mechanical signal and then transformed back to optical signal. It is a new method for preparing visible‐light‐responsive structural color material and has great potential in display devices, anticounterfeiting labels, and data storage.

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