Low-cost preparation of durable electrocatalysts is vital for energy storage and conversion. Here, we integrated two methods of synthesizing isolated iron atoms into a special carbon matrix as an advanced electrocatalyst. Atomic Fe isolation and graphene nanomeshes or curved carbon nanoshells were almost synthesized simultaneously. The hierarchical atomic Fe/carbon material with 0.53 atom % Fe exhibited superior oxygen reduction reaction (ORR) performance to Pt–C (20 wt % Pt) with 40 mV more positive onset potential, larger current density, and stronger methanol-tolerant capability. We demonstrated that the catalytic active sites were Fe isolation and coordinated with nitrogen in the porous curved carbon-graphene matrix. This strategy could be developed into a general approach to prepare atomic metal/carbon electrocatalysts.

Hetero-layered iron–nitrogen coordination between g-C3N4 and graphene nanomeshes was developed for superior electrocatalytic activity in the oxygen reduction reaction.