The focus of this research lies on fundamental research to provide guidelines for the design of new nanocatalyst toward improvement of the performance of proton exchange membrane fuel cells (PEMFCs). To achieve this overarching goal, several specific steps were taken with aims to: (1) provide guidelines for the design of new catalysts; (2) promote nanocatalyst applications towards alternative energy applications; and (3) integrate advanced instrumentation into nanocharacterization and fuel cell (FC) electrochemical behavior. In tandem with these goals, the cathode catalysts were extensively refined to improve the performance of PEMFCs and minimize noble metal usage. In this study, the major accomplishment was producing aligned carbon nanotubes (ACNTs), which were then modified by platinum (Pt) nanoparticles via a post-functionalization colloidal chemistry approach. The Pt-ACNTs demonstrated improved cathodic catalycity, by building better device endurance and decreased Pt loading. It was also determined that surface mechanical properties, such as elastic modulus and hardness were increased. Collectively, these enhancements provided an improved FC device. The electrochemical analyses indicated that the power density of the PEMFCs was increased to 900 mW/cm2 and current density to 3000 mA/cm2, respectively. The Pt loading was controlled at lower than 0.2 mg/cm2 to decrease the manufacturing expenses.