Fortunately, proton exchange membrane fuel cells (PEMFCs) possess the potential of higher energy densities depending on the amount of carried H 2 , which have realized the commercial application in the field of heavy truck and shipping. Oxygen reduction reaction (ORR) is the cathode reaction of PEMFCs. [1][2] Its sluggish kinetics directly hinder the overall efficiency of PEMFCs. Although commercial carbon supported Pt (Pt/C) has been proven to be the most efficient electrocatalysts for ORR, their scarcity, high cost, and poor stability in long-term operations is a huge impediment to the large-scale deployment of PEMFCs. [3] To address these issues, it is urgently needed to reduce the Pt usage simultaneously improving its activity and stability, or ultimately to replace precious metal Ptbased catalysts with non-precious-metal catalysts.An effective strategy to reduce Pt usage is alloying Pt with a second transition metal (M = Fe, Co, Ni, etc.) and further precisely tuning its composition and structure. [4][5][6][7][8][9][10][11][12][13][14] It is reported that structurally ordered intermetallic Pt-M alloys exhibited a significant enhancement on ORR performance. The enhanced performance is attributed to that incorporating M atoms with a smaller atomic radius in the Pt-M alloys provides a compressive strain to Pt atoms on the surface, lowers its d-band center, Lowering noble-metal Pt usage and simultaneously enhancing electrocatalytic oxygen reduction reaction (ORR) activity and stability of Pt-based ORR electrocatalysts is the key to realize the large-scale application of fuel cells. Here, an effective strategy is developed to reduce Pt usage through the strong electron interaction between uniform Pt nanoparticles (≈4.0 nm) and abundant atomically dispersed Fe-N 4 sites modified on an ordered mesoporous carbon (OMC) surface for efficiently enhancing ORR performance. Density functional theory (DFT) calculations show that the strong electron interactions between Pt and Fe-N 4 sites decrease the d-band center of Pt in Pt@Fe-N-OMC-2 by 0.21 eV relative to that of as-prepared Pt@OMC, indicating the weakened O 2 adsorption and accelerated desorption of oxygenated species on Pt sites. In situ Raman spectra demonstrate that the introduction of Fe-N 4 moieties promotes the O-OH dissociation process. Finite element method simulations reveal that the electric and thermal field of the embedded Pt nanoparticle surface is enhanced through modifying Fe-N 4 sites on the OMC surface, accelerating the accumulation of ORR-related species (O 2 , H + , and H 2 O), which is conductive to electrocatalyzing the ORR. This innovative approach not only illustrates the synergistic mechanism between Pt and Fe-N 4 sites, but also simultaneously provides new avenues to design advanced electrocatalysts for fuel cells.