Zn-air batteries (ZABs) stand among the most promising energy devices for a post-lithium-ion battery system due to their high theoretical energy density (1086 Wh/kg), high cell voltage (1.66 V), good safety, low cost, and environmental friendliness. The biggest challenge in developing the high-performance rechargeable ZABs is the design of suitable bifunctional air electrodes with controlled chemical composition and a well-designed architecture for effectively catalyzing the critical oxygen reactions, i.e., oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). The sluggish kinetics of ORR and OER requires bifunctional electrocatalysts in air cathodes to develop high-performance rechargeable ZABs. Pt-based and Ru/Ir oxide-based materials are state-of-the-art electrocatalysts for ORR and OER, respectively. Still, the prohibitive cost and scarce reserve hinder their extensive use. Transition metals (e.g., Co, Fe, Ni, Mn) and nitrogen (N) co-doped carbons (M-N-C) have been widely studied and accepted as promising candidates for ORR catalysts. Their adjustable coordination structures and electronic environments are also favorable for enhancing the OER performance by introducing strategies, i.e., porous structure, heteroatom coordination, dual metal sites, and defect engineering . In this work, an optimization study on the cathode composition and configuration of its different components was carried out to obtain high-performance and easy-to-use cathodes for ZABs. Bifunctional dual metal site FeNiP@FeNC catalysts based on porous organic polymers as soft templates have been developed to replace the state-of-the-art Pt/C-RuO2 for accelerating ORR and OER in rechargeable ZAB.