Herein, Pt nanoparticles supported on a polymer substrate are electrochemically synthesized and used for methanol electrooxidation in alkaline media. The effect of the cocatalyst, supporting materials, and electrodeposition mode on the improvement in the electrocatalytic activity of Pt nanoparticles towards methanol oxidation is investigated. The electrochemical experiments demonstrate that ternary nanoparticles supported on the polymeric substrate through the pulse electrodeposition technique (p-Pt/NiCu/p-MDAB/MWCNT) boost the methanol oxidation reaction (MOR). The MOR enhancement can result from an improvement in the size, dispersion, and porosity of metallic nanoparticles. This study implies that an appropriate selection of the cocatalyst and preparation method is promising for the design and fabrication of profitable electrocatalysis.