“…It thus remains a primarily challenge in realizing high‐power and high‐energy densities in pseudocapacitors, which requires pseudocapacitive electrode materials simultaneously providing large specific surface area and ultrahigh transports of ions and electrons 22, 23, 24. In this regard, controlling nanostructures and exploring novel materials have become critical processes to meet these requirements in developing TMO‐based composite electrodes,1, 6, 17, 23, 25 wherein various conductive materials, including nanostructured carbons (such as porous carbon,14, 26 carbon nanotubes,27, 28, 29, 30 and graphene 31, 32) and conducting polymers, are extensively employed to serve as electron pathways. Although the large specific surface area in these low‐dimensional composite nanostructures allows ion transports,1, 17, 23, 26, 27, 28, 29, 30, 31, 32 their assembled bulk electrodes usually exhibit high electrical resistance as a result of the short electron transport distance within these low‐dimensional conductive materials, the undesirably high contact resistances produced by the coating of electrically insulating active TMOs and polymer binders, as well as the weak and noncoherent TMO/conductor interfaces 24, 33, 34, 35.…”