Abstract Martensitic transformation, usually accompanied by ferroelastic and thermoelastic behaviors, is an interesting and useful mechanical-related property upon external stimuli. For molecular crystals, however, martensitic systems to show reversible stimuli-actuation behaviors are still limited because of a lack of designability and frequent crystal collapse due to large stress releases during the transformations. Here, a one-dimensional hybrid perovskite semiconductor (NMEA)PbI 3 (NMEA =  N -methylethylammonium) was prepared by following a dimensionality reduction design principle. The crystal undergoes reversible ferroelastic and thermoelastic martensitic transformations, which are attributed to weak intermolecular interactions among the chains that easily trigger the interchain shearing movement. The actuation behavior occurring during the phase transition is very close to room temperature and demonstrated to behave as a mechanical actuator for switching. This work provides an effective approach to designing molecular actuators with promising applications in next-generation intelligence devices.