In this paper, a graphene/shape-memory polyurethane (PU) composite film, used for a supercapacitor electrode, is fabricated by a simple bonding method. In the composite, formerly prepared graphene paper is closely bonded on the surface of the PU slice, forming a bi-layered composite film. Based on the good flexibility of graphene paper and the outstanding shape holding capacity of PU phase, the resulting composite film can be changed into various shapes. Also, the composite film shows excellent shape recovery ability. The graphene/PU composite film used as the electrode maintains a satisfactory electrochemical capacitance of graphene material and there is no decay in the specific capacitance after long-cycle testing, making it attractive for novel supercapacitors with special shapes and shape-memory ability.