Targeting high-performance yet cost-effective Pt-based catalysts with low Pt usage and high Pt utilization remains a big challenge in the oxygen reduction reaction (ORR) electrocatalysis. In this work, we demonstrate delicate engineering of strain control via N-doping in ordered PtZn intermetallic nanoparticles supported on N-doped carbon (PtZnN/NC). Benefiting from the ameliorated compressive strain and consequently greatly optimized electronic structures, PtZnN/NC displays ultrahigh ORR activity and durability in both acidic and alkaline media, with respective high mass activities of 297.5 and 80.7 A gPt–1 at 0.9 VRHE, exceeding those of benchmark Pt/C by 8.3- and 2.8-folds. Theoretical calculations reveal that the N-doping effectively lowers the d-band center of PtZnN, resulting in loose binding of *OH on the PtZnN surface, which facilitates the potential-determining step with a reduced energy barrier. This work successfully offers strategic guidance for strain equilibration in alloys via N-doping toward the rational design of advanced electrocatalysts.
