This work illustrates the utility and improved performance of nitrogen-modified catalyst supports for direct methanol fuel cell (DMFC) applications. A unique two-step vapor-phase synthesis procedure is used to achieve the N-modification and Pt-Ru decoration of high surface-area carbon powders relevant to integration as electrocatalysts in fuel cell membrane electrode assemblies (MEAs). First, nitrogen surface moieties are incorporated into a commercial high surface area carbon support via a N-ion implantation technique, followed by Pt-Ru nanoparticle deposition via magnetron sputtering. The nitrogen-ion implantation of high surface area carbon supports yields superior Pt-Ru catalyst particle stability and performance as compared to industry standards. Specifically, results indicate a higher retention of metal catalyst surface area and electrochemical activity after accelerated electrochemical degradation testing. Further, characterization of catalyst materials before, during and after the electrochemical cycling provides insight into the catalyst particle coarsening and/or catalyst surface area loss mechanisms that dominate this fuel cell catalyst system.