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The exploration of direct and effective strategies to construct catalysts with targeted active sites is highly desired. Herein, we report a self-template strategy to fabricate Cu/Fe dual-metal-atoms active sites anchored on MOF-derived porous carbon nanosheets (Cu/Fe/N–CNS). Well-defined Cu/Fe/N–CNS performs outstanding electrocatalytic ORR activity with half-wave potential (0.91 V) in alkaline solution, which outperforms commercial Pt/C catalyst. DFT computational studies indicate that Fe–N active sites on Cu/Fe/N–CNS are more favored than Cu–N active sites for the activation of O–O-containing intermediate products to further boost electrocatalytic activity. Furthermore, Cu/Fe/N–CNS exhibits superior discharge stability with negligible voltage fading over 20 cycles (∼150 h) at 15 mA cm−2 in primary Zn-air batteries. This strategy can open new avenues for the construction of superb dual-metal catalysts. ....