A one-step soft-template induced strategy is demonstrated for the controlled synthesis of nitrogen-enriched core–shell structured cobalt−carbon nanoparticles (NPs) sequentially aligned on wrinkles of N-doped carbon nanosheets (Co-C@NWCs). The key feature of Co-C@NWCs for ORR catalysis enhancement is that it combines high catalytic centers of Co-C core–shell NPs with the wrinkle of carbon nanosheets with high electron donation ability.