Flexible energy storage devices 1Ϫ3 have many potential applications in portable electronic devices, 4Ϫ6 including roll-up display, electronic paper, stretchable integrated circuits, and wearable systems for personal multimedia, computing, or medical devices. Flexible supercapacitors are available with large power density, moderate energy density, good operational safety, and long cycling life and hence are highly desirable as a modern energy storage system. 7 A freestanding binder-free electrode with favorable mechanical strength and large capacitance is a vital component of a flexible supercapacitor. Although transition metal oxides and conducting polymers have been widely studied as supercapacitor electrode materials, only carbon-based materials have shown favorable flexibility and hence been promising as freestanding soft electrodes. Papers, films, and/or clothes made from carbon nanotubes/fibers have been demonstrated to be suitable as freestanding electrodes.2,8Ϫ13 Nevertheless, the less active surface of carbon materials always prevents them from high capacitance performance. The incorporation of an electrochemically active second phase in a carbonbased freestanding electrode can dramatically enhance the electrode capacitance.14 Graphene is an intriguing twodimensional carbon material and has attracted much research attention due to several breakthroughs in fundamental research and promising practical applications.
15Ϫ30Chemical modified graphene exhibits enormous active edges and oxygen functional groups. It has extraordinary electrochemical and mechanical properties comparable to or even better than carbon nanotubes. 21,26,27 Flexible papers with graphene sheet or graphene oxide sheet as sole building block have already been fabricated by flow-directed assembly. 16,25,31,32 Graphene paper presents excellent tensile modulus up to 35 GPa and room temperature electrical conductivity of 7200 S m
Ϫ1. 25 These intriguing characteristics enable graphene paper as a freestanding electrode. Various conducting polymers have been widely studied as electrode materials for supercapacitors because of their high capacitance, easy production, and low cost. However, poor conductivity and weak flexibility of conducting polymers limit them from usage in high-performance flexible supercapacitors. It has been confirmed that graphene can enhance not only the electric conductivity of silica 18 but especially the mechanical strength of polymer composites. 21 This work is aimed to prepare graphene-conducting polymer composite paper as a flexible electrode combining the advantages of graphene paper (high