Over the past years numerous research groups in both academia and industry around the world have consciously increased efforts to design and develop advanced materials with dimensions ranging from a few to several hundred nanometers. Their motive is that the physical and chemical properties of the nanoscopic substances can differ considerably from the properties exhibited by the same materials in the bulk.[1] Recently, nanostructured electrode materials have attracted great interest, as they show better rates and capabilities than traditional materials. With nanostructured electrode materials, the distance within the material over which the electrolyte must transport ions is dramatically smaller than with conventional electrodes composed of chemically similar bulk materials. [2][3][4][5] Hence, advanced materials with nanostructure have been studied widely as the electrode materials of energy-storage devices (for example batteries and, especially, supercapacitors).[6]Electrochemical capacitors combining the advantages of the high power of dielectric capacitors and the high specific energy of rechargeable batteries have played an increasingly important role in power source applications such as hybrid electric vehicles and short-term power sources for mobile electronic devices. [7,8] Nowadays, much research on electrochemical capacitors is aimed at increasing power and energy density as well as lowering fabrication costs while using environmentally friendly materials. Some transition metal oxides, such as RuO 2 and IrO 2 , exhibit prominent properties as pseudocapacitive electrode materials. The highest value for specific capacitance reported for amorphous hydrated RuO 2 is 840 F g -1 .[2,9] However, despite the remarkable performance of this material, its high cost excludes it from wide application. Although some low-cost metal oxides (such as MnO 2 or NiO) and conductive polymers also exhibit electrochemical capacitance behavior to some extent, their capacitance performances are much poorer than that of RuO 2 . Among these materials, polyaniline (PANI) has been considered as one of the most promising materials for electrode materials in redox supercapacitors because of its low cost, ease of synthesis, and relatively high conductivity. However, its capacitance value is much less than that of RuO 2 . It is well known that, in pseudocapacitive electrode materials, the pseudocapacitance is mainly produced by the fast faradaic reaction occurring near a solid electrode surface at an appropriate potential.[10] Therefore nanostructured materials can provide a relatively short diffusion path to improve the utilization of supercapacitor electrodes at high power density. Over the years, different morphologies of PANI have been obtained by changing the synthesis method. Nanotubes or nanofibers of PANI have been synthesized by using a porous membrane template.[11] By using the template-directed synthesis method, a unique and ordered structure can be built up directly, but post-processing is required in order to remove the te...