Platinum nanoparticles with continuously tunable mesoporous structures were prepared by as imple,o ne-step polymeric approach. By virtue of their large pore size, these structures have ahigh surface area that is accessible to reagents. In the synthetic method, variation of the solvent composition playsanessential role in the systematic control of pore sizeand particle shape.T he mesoporous Pt catalyst exhibited superior electrocatalytic activity for the methanol oxidation reaction compared to commercially available Pt catalysts.T his polymeric-micelle approach provides an additional design concept for the creation of next generation of metallic catalysts.Micelle architectures provide as imple and versatile platform for the synthesis of mesoporous structures in aw ide variety of materials. [1] Both pore size and the porous structure of the materials can be controlled by tuning the inter-a nd intramolecular forces that drive the self-assembly of surfactants and block copolymers. [2] Mesoporous materials with large pore sizes have inspired aw ide variety of applications because large pores facilitate fast and efficient transport of reactants. [3] Forexample,Zhao and co-workers reported that three-dimensional (3D) ordered mesoporous silica with ultralarge accessible mesopores can be synthesized on highmolecular-weight block-copolymer templates.T hey used solvent evaporation to make composite micelles composed of ab lock copolymer and as ilica precursor to assemble the ordered mesostructure. [4] Although the synthesis of these large-pore materials have been demonstrated, their compositions are still limited to carbon, [5] silica, [4,6] metal oxides, [7] and organosilicates. [8] If these micelle templates could be applied to the preparation of noble metals,i np articular, materials such as platinum, these ultralarge accessible surfaces would be of great utility for electrocatalysis.Mesoporous noble-metal materials (e.g.,A u, Pt, Pd) have most of the physical and chemical properties that make these metals good catalysts.C onsequently,t hese structures exhibit enhanced catalytic properties for ar ange of reactions, including small-organic-molecule oxidation, the oxygen reduction reaction, and hydrogenation. [9] Our previous studies demonstrated that mesostructured noble metals with large pores could be synthesized by using pore-directing agents, such as the block copolymer polystyrene-block-poly(ethylene oxide) (PS-b-PEO), through electrochemical deposition. [10] However,t his method required the metal species to be electrodeposited on conductive substrates,l imiting the obtained materials primarily to monolith films.C hemical reduction might provide am ore flexible way to make metal nanoparticles in solution. [11] To our knowledge,c hemical reduction has never been used for the controlled synthesis of large-sized porous metallic nanoparticles with tunable pore sizes and particle sizes.Consequently,new synthetic strategies must be developed to enable the reduction of metal species on block-copolymer micelles to creat...