▎ 摘　　要

A general layered- template strategy has been developed to construct graphene-like Fe-N-C nanosheets (g-FeN-CNS) by lamellar confinement of layered clay montmorillonite (MMT) using iron complexes as precursors. During pyrolysis, iron complexes could be transformed into atomically dispersed Fe and N co-doped carbon nanosheets in the interlayer space of MMT. After removing the MMT template, the as-fabricated g-Fe-N-CNS exhibited excellent ORR performance with a more positive halfwave potential (E-1/2) of 0.87 V, good stability, and superior methanol tolerance. Furthermore, g-Fe-N-CNS assembled as the air cathode also exhibits encouraging performance in the primary Zn-air batteries. These excellent ORR performances are ascribed to the high specific surface area, hierarchically mesoporous structure, unique 2D nanosheet architecture, and uniformly dispersed Fe-N active sites. Besides, the calculation results indicate that with the ORR process on Fe-N active sites, the adsorption of *OOH is the most crucial step in determining the reaction rate on g-Fe-N-CNS. This layered-template approach provides a general synthetic methodology toward 2D heteroatom-doped carbon nanosheets for highly efficient energy conversion.