There is an urgent demand for developing highly efficient bifunctional electrocatalysts with excellent stability toward the oxygen evolution and reduction reactions (OER and ORR, respectively) for rechargeable Zn-air batteries (ZABs). In this work, NiFe nanoparticles encapsulated within ultrahigh-oxygen-doped carbon quantum dots (C-NiFe) as bifunctional electrocatalysts are successfully obtained. The accumulation of carbon layers formed by carbon quantum dots results in abundant pore structures and a large specific surface area, which is favorable for improving catalytic active site exposure, ensuring high electronic conductivity and stability simultaneously. The synergistic effect of NiFe nanoparticles enriched the number of active centers and naturally increased the inherent electrocatalytic performance. Benefiting from the above optimization, C-NiFe shows excellent electrochemical activity for both OER and ORR processes (the OER overpotential is only 291 mV to achieve 10 mA cm-2). Furthermore, the C-FeNi catalyst as an air cathode displays an impressive peak power density of 110 mW cm-2, an open-circuit voltage of 1.47 V, and long-term durability over 58 h. The preparation of this bifunctional electrocatalyst provides a design idea for the construction of bimetallic NiFe composites for high-performance Zn-air batteries.