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Single‐atom catalysts (SACs) with highly active sites atomically dispersed on substrates exhibit unique advantages regarding maximum atomic efficiency, abundant chemical structures, and extraordinary catalytic performances for multiple important reactions. In particular, M–N–C SACs (M=transition metal atom) demonstrate optimal electrocatalytic activity for the oxygen reduction reaction (ORR) and have attracted extensive attention recently. Despite substantial efforts in fabricating various M–N–C SACs, the principles for regulating the intrinsic electrocatalytic activity of their active sites have not been sufficiently studied. In this Review, we summarize the regulation strategies for promoting the intrinsic electrocatalytic ORR activity of M–N–C SACs by modulation of the center metal atoms, the coordinated atoms, the environmental atoms, and the guest groups. Theoretical calculations and experimental investigations …