Electrocatalytic　oxygen　reduction　reaction　(ORR)　for　H2O2　production　presents　an　alternative　approach　suitable　for　on-site　applications.　Although　atomically　dispersed　earth-abundant　metal　species　anchored　in　a　nitrogen-doped　carbon　framework　(M–N–C)　have　demonstrated　significant　2e−　ORR　activity,　the　Ni–N–C　catalyst　exhibits　unfavorable　catalytic　activity.　It　is　well-recognized　that　the　d-band　center　of　the　metal　can　be　tailored　by　introducing　transition　metals,　thereby　altering　the　adsorption　free　energy　of　the　OOH∗　reactive　species.　Herein,　we　have　designed　a　dual-single-atom　configuration　(Ni–ZnNC),　where　the　Zn　atom　serves　as　a　modulator　to　adjust　the　d-band　electronic　energy　of　the　Ni　center,　ultimately　optimizing　the　intermediate　adsorption　and　resulting　in　high　2e−　ORR　performance.　The　Ni–ZnNC　catalyst　demonstrates　an　H2O2　production　rate　of　5.6　mol/g/h　at　0.0　VRHE　with　a　notable　H2O2　selectivity　of　approximately　60%　in　an　acid　electrolyte.　Density-functional　theory　calculations　reveal　that　the　Zn　atom　effectively　alters　the　d-band　electronic　energy　of　the　Ni　center,　strengthening　the　Ni–OOH∗　binding　affinity　and　thereby　enhancing　the　adsorption　process.　This　work　provides　valuable　insights　into　the　design　of　earth-abundant　metal　Ni-based　electrocatalysts　for　H2O2　generation.　©　2023　Elsevier　Ltd