Developing OER&ORR bifunctional electrocatalysts has great significance for promoting the green energy conversion and storage technologies. Herein, nitrogen doped carbon coupled FeNi3 intermetallic compound (FeNi3@NC) is designed and constructed by a super facile route. Rich defects, multiple active centers and strong synergistic effect allow FeNi3@NC with superior OER&ORR performance in alkaline environments. It exhibits an ultralow overpotential (Eover) of 277?mV at 10?mA/cm2 for OER, and a high half-wave potential (E1/2) of 0.86?V for ORR which outperform commercial Pt/C electrocatalysts. As a result, the ΔE (ΔE?=?Eover,OER – E1/2,ORR) value of 0.65?V largely surpasses Pt/C-IrO2 noble metal benchmarks (ΔE?=?0.73?V). Furthermore, density function theory calculations are performed to probe its electrocatalytic mechanism. As expected, the peak power density and energy density of FeNi3@NC based rechargeable Zn-air battery reaches 139?mW/cm2 at 234?mA/cm2 and 915 Wh kg-1 at 10?mA/cm2, respectively, with excellent stability. Our exploration provides a guideline for synthesis of advanced bifunctional electrocatalyst.