Among metal-air batteries, especially for aqueous zinc-air batteries (ZABs), have recently attracted increasing attention, due to their advantages with respect to the abovementioned shortcomings of the LIB, for example, their five-times higher (1086 W h kg −1 ) specific energy density, lower manufacturing cost (≈10$ kW −1 h −1 ), and lower toxi city and intrinsic safety derived from the aqueous property. [18][19][20][21][22] Generally, ZABs are composed of four parts, the air electrode, electrolyte, separator, and Zn metal electrode. As the main reactions on air electrodes during charging/discharging processes, oxygen evolution/reduction reactions (OER/ ORR) are usually limited by their sluggish kinetics, resulting in higher overpotential, unsatisfactory energy efficiency, lower power density, and poor cycling stability, all of which could severely restrict the commercialization of ZABs. Thus, to deal with this situation, great efforts have been afforded to developing highly efficient oxygen electrocatalysts with lower costs.Noble-metal-based materials (Ru, Pt, Ir, and their alloys) have usually been considered as the benchmark of advanced electrocatalysts, owing to their strong catalytic ability toward the ORR and OER, but unfortunately, their high prices have hindered their wide and large-scale application. Recently, Fe-based singleatom catalysts (SACs) and dual-atom catalysts (DACs) have attracted great attention. Compared with other transition metalbased SACs, such as Co, Ni, and Mn, experimental results and theoretical calculation has been confirmed that the Fe-N structure possessed highest ORR activity and outstanding OER performance due to the appropriate adsorption/desorption energy of the oxygen-containing intermediates during the catalytic procedure. [23,24] Besides, with regard of general Fe-C moiety and Fe cluster, Fe-N structure not only displayed lower kinetics barrier owing to the reduced free energy for the step from O* to the OOH*, but also the firm connection between Fe atoms and N atoms could take the responsibility for their better catalytic stability. [25] Based on those advantages, the Fe-N x has laid a solid foundation of serving as bifunctional oxygen electrocatalysis, offering a promising strategy to construct effective air electrodes of ZABs (Figure 1). [26][27][28][29][30][31] In 2017, Chen et al. successfully anchored atomically dispersed Fe-N x on S-doped hierarchical carbon layers and were the first applied to ZABs. [32] Benefitting from the abundance of single-atom active sites, the uneven charge distribution caused by the N and S codopants, and its outstanding electrical conductivity, the electrocatalyst showed Pt-like performance toward the OER (η 10 , the overpotential at a As one of the most competitive candidates for large-scale energy storage, zincair batteries (ZABs) have attracted great attention due to their high theoretical specific energy density, low toxicity, high abundance, and high safety. It is highly desirable but still remains a huge challenge, however, to achieve ...