Pursuing　effective　and　generalized　strategies　for　modulatingtheelectronic　structures　of　atomically　dispersed　nanozymes　with　remarkablecatalytic　performance　is　exceptionally　attractive　yet　challenging.Herein,　we　developed　a　facile　＂formamide　condensation　and　carbonization＂strategy　to　fabricate　a　library　of　single-atom　(M-1-NC;6　types)　and　dual-atom　(M-1/M-2-NC;　13　types)metal-nitrogen-carbon　nanozymes　(M　=　Fe,　Co,　Ni,　Mn,　Ru,　Cu)　to　revealperoxidase-　(POD-)　like　activities.　The　Fe1Co1-NC　dual-atom　nanozyme　with　Fe-1-N-4/Co-1-N-4　coordination　displayed　the　highest　POD-like　activity.Density　functional　theory　(DFT)　calculations　revealed　that　the　Coatom　site　synergistically　affects　the　d-band　center　position　of　theFe　atom　site　and　served　as　the　second　reaction　center,　which　contributesto　better　POD-like　activity.　Finally,　Fe1Co1　NC　was　shown　to　be　effective　in　inhibiting　tumor　growth　both　in　vitro　and　in　vivo,　suggesting　that　diatomicsynergy　is　an　effective　strategy　for　developing　artificial　nanozymesas　novel　nanocatalytic　therapeutics.