The successful commercialization of the direct methanol fuel cell (DMFC) is inseparable from the development of advanced Pt-based anode catalysts with high electrocatalytic activity and acceptable manufacturing cost. Here, we present a robust bottom-up strategy to anchor ultrasmall Pt nanocrystals with an average diameter of only 2.3 nm onto carbon nanohorn-decorated three-dimensional (3D) graphene networks (Pt/CNH-G) through a controllable self-assembly process. The as-derived 3D Pt/CNH-G catalysts manifest a series of distinctive architectural advantages, such as interconnected porous frameworks, large accessible surface areas, plentiful active cones, highly dispersed Pt nanoparticles, and good electron conductivity. Consequently, the optimized Pt/CNH-G catalyst is endowed with exceptional methanol oxidation properties with a large electrochemical active surface area of 128.6 m2 g-1, a high mass activity of 1626.0 mA mg-1, and excellent long-term stability, which are significantly superior to those of conventional Pt catalysts supported by carbon black, carbon nanotube, carbon nanohorn, and graphene matrices.