The performance of electrochemical energy storage devices relies largely on a scrupulous design of nanoarchitectures and smart hybridization of active materials. Nanoarray electrodes are particularly investigated for power source in microelectronics, which requires high rates, high areal capacity/capacitance and long cycle stability. When the metal-ion battery electrode materials are designed into nanostructures (e.g., 1D array, 2D nanosheets), the pseudocapacitive effect may become dominating and can boost the high-rate performance. Our group has been actively working on nanoarray materials directly on conductive substrates as electrodes for Li-ion and Na-ion storage. In this talk, I will articulate our material design strategies and how the extrinsic pseudocapacitance effect contributes to the high-rate performance. This effect applies to intercalation, conversion, as well as alloy type electrodes. These materials include VO2, SnS, and MoSeS. Full hybrid batteries (or called Li-ion or Na-ion capacitors) will also be presented based on such subtle designed electrodes.