Mesoporous SBA-15 silica materials functionalized with and without carboxylic acid groups were used to effectively control the morphology of Pt crystals, and the materials thus obtained were applied to methanol oxidation reactions. The Pt particles aggregated to form long spheroids inside the channels in pure SBA-15. When carboxylic acid groups were utilized, the SBA-15(-COOH) material facilitated the formation of higher Pt surface area, smaller Pt nanoparticles and nearly spherical shape due to the strong interaction between Pt4+ ions and carboxylic acid on SBA-15. The Pt4+ ions on the SBA-15(-COOH) material can be directly transformed to reduced Pt particles during calcination. The methanol oxidation activity on a Pt surface is strongly dependent on the shape of Pt particles. The near-spherical Pt nanoparticles on the SBA-15(-COOH) exhibited higher catalytic activity during methanol oxidation than Pt catalysts on unmodified SBA-15. The near-spherical Pt particles on the SBA-15(-COOH) contained large numbers of terrace sites on their surfaces, which led to high efficiency during methanol oxidation.