Carbon‐wrapped Co/Ni metal nanoparticles (C@Co
xNi1−x) were synthesized by calcination of bimetallic metal–organic frameworks (Co/Ni‐MOFs), prepared by a hydrothermal reaction, under N2 atmosphere and explored as bifunctional catalysts for oxygen reduction reactions (ORR) and oxygen evolution reactions (OER) for rechargeable Zn‐air batteries. Linear sweep voltammetry (LSV) measurements indicated that the composite obtained at 600°C (N600) exhibited superior electrochemical performance to other composites obtained at 500, 700, 800, and 900°C, respectively. Also N600 exhibited stable current–voltage profiles in a cycling test conducted in 8 M KOH solution for 200 h, suggesting that N600 can be a potential catalyst for rechargeable Zn‐air batteries.