Artificial superlattice nanocomposites are successfully prepared by electrostatic heteroassembly of redoxable Co-Al or Co-Ni layered double hydroxide (LDH) nanosheets with graphene. The superlattice electrodes exhibit a high capacity up to ca. 650 F/g, which is approximately 6 times that of pure graphene. The composites are found to be capable of superfast charging and discharging, up to ca. 100 Hz, comparable with the high-power performance of graphene electrodes.