It is critically important to develop actuator systems for diverse needs ranging from robots and sensors to memory chips. The advancement of mechanical actuators depends on the development of new materials and rational structure design. In this study, we have developed a novel graphene electrochemical actuator based on a rationally designed monolithic graphene film with asymmetrically modified surfaces. Hexane and O(2) plasma treatment were applied to the opposite sides of graphene film to induce the asymmetrical surface properties and hence asymmetrical electrochemical responses, responsible for actuation behaviors. The newly designed graphene actuator demonstrated here opens a new way for actuator fabrication and shows the potential of graphene film for applications in various electromechanical systems.