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The hierarchical nanoporous (NP) PtFe alloy with multimodal size distributions is straightforwardly fabricated by means of mild de-alloying of the PtFeAl source alloy. This interesting NP structure consists of interconnected larger ligaments around hundreds of nanometers, in which these ligaments are also composed of the three-dimensional network structure with the typical size at 3 nm. In comparison to NP-Pt and Pt/C catalysts, the as-made alloy nanostructure exhibits superior electrocatalytic activity for the methanol oxidation reaction (MOR) with higher catalytic durability and CO tolerance besides the enhanced specific and mass activity. NP-PtFe also shows improved structure stability with the less loss of the electrochemical surface area of Pt upon long-term potential scan in acidic solution. X-ray photoelectron spectroscopy and density functional theory calculations demonstrate that the incorporation of Fe appropriately modified the electron structure of Pt with the downshift of the Pt d-band center, leading to a decreased CO poisoning and an improved MOR activity.