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Proton exchange membrane fuel cells require electrocatalysts with a high platinum (Pt) loading, large active surface area, and favorable hydrodynamic profile for practical applications. Here, we report the design of three-dimensional hierarchical bimodal macroporous carbon nanospheres with an interconnected pore system, which are applied as an electrocatalyst support. Carbon-supported Pt (Pt/C) catalysts were prepared by aerosol spray pyrolysis followed by microwave chemical deposition. The hierarchical porous structures not only increased the dispersion of Pt nanoparticles but also improved catalytic performance. A hierarchical bimodal macroporous Pt/C catalyst with a mixture of 30 and 120 nm size pores showed the best performance. The electrochemical surface area and mass activity values of this support were 96 m² g^–1-Pt and 378 mA mg^–1-Pt, respectively at a Pt loading of 15 wt %.