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Developing metal-free carbon electrocatalysts with atomically precise structures of hetero-doping is crucial for inventing reliable alternatives to precious metal-based catalysts. Our study reveals that the optimal active site is the edge-exposed N-neighbored carbon site in a chained N- C -C-S structure. Carbon material with N- C -C-S functional doping is controllably synthesized through polymer dehalogenation and heteroatom doping with thiomorpholine at room temperature. The resulting N/S-co-doped carbon with N- C -C-S functionalization, named N-C 2 -S, exhibits excellent ORR performance compared to other types of N, S-co-doped carbon, and commercial Pt/C. Typically, the N-C 2 -S sample shows the earliest onset potential of 0.96 V and a high half-wave potential of 0.85 V for promoting ORR. Assembled into an Al-air battery, The N-C 2 -S delivers an exceptional open-circuit voltage of 1.95 V and a large specific power of 128.1 mW cm 2. The synthesis strategy developed in this work can potentially open up precise functionalization of synthetic carbons with heteroatoms. [Display omitted] • The C site near the N in N-C-C-S is identified as highly active for oxygen reduction. • Different types of N, S-co-doped carbon are obtained via dehalogenation of PVDC. • N-C-C-S doping is realized via dehalogenation coupling reaction with thiomorpholine. • The N-C 2 -S sample exhibits exceptionally good oxygen reduction reaction performance. • The N-C 2 -S-assembled Al-air battery delivers high cell voltages and large powers. [ABSTRACT FROM AUTHOR]