Limited by the sluggish four-electron transfer process, designing high-performance nonprecious electrocatalysts for the oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) is urgently desired for efficient rechargeable Zn-air batteries (ZABs). Herein, the successful synthesis of porous nitrogen-doped cobalt pyrite yolk-shell nanospheres (N-CoS 2 YSSs) is reported. Benefiting from the abundant porosity of the porous yolk-shell structure and unique electronic properties by nitrogen doping, the as-prepared N-CoS 2 YSSs possess more exposed active surface, thus giving rise to superior activity for reversible oxygen electrocatalysis and outstanding cycling stability (more than 165 h at 10 mA cm −2) in ZABs, exceeding the commercial Pt/C and RuO 2 hybrid catalysts. Moreover, the assembled ZABs, delivering a specific capacity of 640 mAh g Zn −1 , can be used for practical devices. This work provides a novel tactic to engineer sulfides as high efficiency and promising bifunctional oxygen electrocatalysts for advanced metal-air batteries. Oxygen electrocatalysis has received widespread attention due to its importance in fuel cells, water splitting, and metal-air batteries. [1-4] Among these sustainable energy storage and conversion technologies, Zn-air batteries (ZABs) have been recognized as a promising global portfolio storage technology due to their unique half-open systems, significant theoretical energy density (1086 Wh kg −1 , including oxygen), much flatter operating voltage (1.66 V), environmental benignity, and good safety. [3,5] However, the sluggish kinetics of oxygen evolution reaction (OER) for charging and oxygen reduction reaction (ORR)