The development of robust and efficient trifunctional catalysts showing excellent oxygen evolution reaction (OER), oxygen reduction reaction (ORR) and hydrogen evolution reaction (HER) kinetics has been challenging. Herein, we prepared a hybrid iron and cobalt-based metal alloy phosphide on a phosphorus and nitrogen co-doped carbon substrate (FeCo-P/PNC) as a catalyst using a one-step Pregulation method. The catalyst exhibited a positive half-wave potential of 0.86 V versus the reversible hydrogen electrode (RHE) for ORR, and low overpotentials of 350 and 158 mV for OER and HER, respectively, to achieve a current density of 10 mA cm −2 . Density functional theory calculations demonstrated the dominant role of P in both FeCo phosphide and carbon matrix, which led to the good ORR, OER and HER kinetics. The assembled aqueous and flexible Zn-air batteries with FeCo-P/PNC as the air cathode displayed excellent peak power densities of 195.1 and 90.8 mW cm -2 , respectively, as well as outstanding charging-discharging performance, long lifetime, and high flexibility. Moreover, the self-powered overall water-splitting cell exhibited a low working voltage of 1.71 V to achieve a current density of 10 mA cm −2 , confirming its excellent multifunctional OER/ORR/HER activity.