The electrochemical deposition of Pt nanoparticles on carbon nanotubes (CNTs) supports and their catalytic activities formethanol electro-oxidation were investigated. Pt catalysts of 4~12nm average crystalline size were grown on supports bypotential cycling methods. Electro-plating of 12min time by potential cycling method was sufficient to obtain smallcrystalline size 4.5nm particles, showing a good electrochemical activity. The catalysts’ loading contents were enhanced byincreasing the deposition time. The crystalline sizes and morphology of the Pt/support catalysts were evaluated using X-ray Diffraction (XRD) and Transmission Electron Microscopy (TEM). The electrochemical behaviors of the Pt/support catalystswere investigated according to their characteristic current-potential curves in a methanol solution. In the result, theelectrochemical activity increased with increased plating time, reaching the maximum at 12min, and then decreased. Theenhanced electroactivity for catalysts was correlated to the crystalline size and dispersion state of the catalysts.