In an attempt to provide a favorable active material of Li+ supercapacitor for HEV use, we modified the surface of an activated carbon fiber felt by coating with some transition metal oxides after mild-oxidation treatment. Major source of enhancing capacitance is attributed to be due to the nano-ionics mechanism proposed by Maier and coworkers. Cyclic voltammetry and constant current charge–discharge performance were examined for the surface modified samples in view of power capability. The oxides of Ag, Cu, Pd, and Sn were found effective to enhance the capacitance and high rate charge/discharge performance. The cycleability test was performed as well.