Nitrogen‐doped carbon has great potential in lithium‐ion batteries (LIBs) and sodium‐ion batteries (SIBs), considering N‐doping can not only improve the surface wettability of carbon materials, but also accelerate charge transfer by generating additional defects. However, designing carbon materials with a high nitrogen content and uniform distribution using conventional doping methods remains a challenge. In this study, a hollow carbon sphere with an ultrahigh nitrogen content of 9.58 wt % was successfully fabricated by rationally designing Schiff base chemistry (PTA‐NHCS‐700). Stable hierarchical pore structures, moderate defects, and large specific surface areas were formed during the carbonization process. Excellent electrochemical performance was observed in LIBs (204.2 mAh g−1 after 7000 cycles at 5 A g−1) and SIBs (154.2 mAh g−1 after 10000 cycles at 5 A g−1). This study not only promotes the development of efficient carbon anode materials for LIBs and SIBs, but also provides a novel idea for the doping of heteroatoms with special chemical structures.

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