The coordination environment of atomic metal sites in single atom catalysts is of vital significance in tailoring the d-orbital states and thus the catalytic behavior towards oxygen reduction reaction (ORR), thereby offering great promise to boost activity via regulating the local chelation structure. Herein we designed a carbon coordination environment for the atomic M sites reside on the right leg of the volcano plot, to effectively counter balance the low adsorption energy of the metal center to oxygen species. Combining time-of-flight secondary ion mass spectrometry and density functional theory calculations, we unveiled the M-C coordination structure and the thus induced changes in electronic structure and ORR catalytic behavior. The reshape in coordination structure, i.e., the replacement of typical nitrogen coordination by low electronegativity carbon coordination, gives rise to exceptional intrinsic activity towards ORR. This work brings a new perspective to boost the activity of single atom catalysts on the weak bonding leg, with exceptional ORR activity being further expected through advancing the chelation structure.