AbstractIn recent years, solvent‐driven actuators have been capable of controlling deformations in response to external stimuli. However, a magnetic polydimethylsiloxane (PDMS) composite film with magnetic properties is traditionally developed using the micro‐electro‐mechanical system process. Although it has general actuation deformation, the composite film suffers from the problems of actuation and control. Here, this is done by co‐mixing PDMS and ferrosoferric oxide (Fe3O4) then waiting for curing and then undergoing ultraviolet‐ozone (UVO) surface treatment. By adjusting the time and orientation of the UVO treatment, a series of solvent‐driven actuators with multiform steady‐state structures (e.g., mono/bistable helix) is proposed. In addition, the deformation of the composite film under different geometrical parameters and surface constraints was visually predicted by incorporating finite element analysis methods. In addition, the controlled deformations of the composite film (such as box‐like, folded, and so on) are carried out by self‐morphing design. Finally, four bionic applications are also proposed to demonstrate the practical use of soft actuators based on Fe3O4‐PDMS films in bionic robots. This work provides new strategies for designing and fabricating programmable and controllable soft actuators and lays the foundation for a wide range of smart material applications.