The first example of a smart crystalline material, the 2:1 cocrystal of probenecid and 4,4'-azopyridine, which responds reversibly to multiple external stimuli (heat, UV light, and mechanical pressure) by twisting, bending, and elastic deformation without fracture is reported. This material is also able to self-heal on heating and cooling, thereby overcoming the main setbacks of molecular crystals for future applications as crystal actuators. The photo- and thermomechanical effects and self-healing capabilities of the material are rooted in reversible trans-cis isomerization of the azopyridine unit and crystal-to-crystal phase transition. Fairly isotropic intermolecular interactions and interlocked crisscrossed molecular packing secure high elasticity of the crystals.