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The development of highly efficient oxygen catalysts is crucial for improving the storage capacity and stability of Li‐O2 batteries. Herein, we report a simple engineering method to prepare the composite electrocatalyst of the CoNi alloy nanoparticles anchored on the N‐doped porous carbon substrate (CoNi/NC), which exhibits the enhanced electrocatalytic performance for the Li‐O2 batteries due to the synergetic effect between the bimetal CoNi alloy and the N‐doped porous carbon framework. The porous structure can expose more active sites, enhance the mass transfer, and temporarily store the Li2O2 intermediate. The CoNi/NC catalyst makes the batteries show a high discharge capacity of 17783 mA h g−1, a low overvoltage of 1.03 V, and long cycle life of 194 cycles. These results indicate that such a simple engineering preparation method can benefit the large‐scale production of high‐efficiency and cost‐effective electrocatalysts for energy applications.

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