Adaptive crystals have attracted significant attention from solid-state chemists and crystal engineers for their promising applications in memories, capacitors, sensors, and actuators. Among them, thermosalient crystals are particularly favored thanks to their efficient energy conversions and rapid responses. However, the mechanisms for the mechanical responses of thermosalient crystals remain largely unclear. Herein we demonstrate that thermosalient effects of molecular crystals could be driven by thermoelastic twisting behaviors. The crystal, based on a model compound with rigid dibenzothiophene sulfone planes and flexible ethoxy chains, can spontaneously self-heal from mechanical fractures. Upon heating, the crystal undergoes remarkable thermosalient behaviors driven by a distinctive left- or right-handed twisting. This thermoelastic twisting converts thermal energy into elastic potential energy, which is further released as kinetic energy upon untwisting to drive the crystal jump. Our demonstration on thermoelastic twisting–induced crystal jumping offers a different perspective on the origins of thermosalient crystals and could provide inspiration for future engineering and application of dynamic molecular crystals.