An innovative elastic crystal based on barbituric acid derivatives (HBDT), which uniquely alters its fluorescence intensity under light exposure is developed. This crystal exhibits significant bending under 365 nm, 450 nm, white light, and sunlight while retaining its elasticity post‐bending. The photomechanical effect of this crystal is driven by intermolecular [2+2] cycloaddition reactions, resulting in light‐activated fluorescence enhancement. These properties open new avenues for applications in robotic arms, information identification, and optical waveguides, presenting a groundbreaking approach for sustainable and flexible crystal applications in material science and optical technology.