Facile synthesis of highly efficient non-precious metal electrocatalysts is intriguing as these catalysts are used in the oxygen reduction reaction (ORR). Herein, we describe an effective protein-mediated approach to access atomically dispersed iron electrocatalyst (Fe SAs/NC) with enhanced accessible metal active sites. This Fe catalyst achieves an exceptional ORR activity in the pH-universal range, especially in alkaline and acid electrolytes with half-wave potentials of 0.94 and 0.84 V (vs RHE), respectively. The unique electronic structure of Fe sites with enhanced electron/proton transportation ability contributes to the optimized adsorption/desorption of oxygen intermediates. In addition, it shows robust durability and excellent tolerance to methanol crossover in pH-universal media. Impressively, it displays encouraging performance when employed in a zinc-air battery, demonstrating a peak power density of 275.1 mW/cm 2 and a specific capacity of 753.8 mAh g −1 . The extremely long-term operational stability of more than 250 h further provides significant potential for its application. • Fe single atoms supported over nitrogen-doped carbon was created. • DFT calculations reveal the support can provide anchoring sites for Fe atoms. • This catalyst shows high catalytic efficacy in oxygen reduction reaction. • The high catalytic activity stems from electronic metal-support interaction.