We report a facile electrochemical method to produce functional groups on the carbon surface in which multiple cyclic voltammetric (CV) sweeps are imposed in 0.5 M H2SO4 electrolyte on the samples containing carbon cloth, Vulcan XC72R, and Nafion ionomer. With supply of ambient O 2, the generation of radicals from the oxygen reduction and Nafion ionomer degradation enables an accelerated formation of oxygenated functional groups on the carbon surface. Raman analysis reveals structural variation for the carbon electrodes after CV modifications. X-ray photoelectron spectroscopy confirms the alteration of carbon structure in conjunction with notable increase of oxygenated groups and reduction in fluorine amount. The functionalized electrodes allow a 250% increment for PtRu electrodeposition as compared to the reference sample. We carry out electrochemical measurements on methanol electro-oxidation for the PtRu samples. The functionalized electrode demonstrates significant improvement in apparent current density and mass activity as opposed to the reference sample.