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Most reported carbonaceous anodes of potassium‐ion batteries (PIBs) have limited capacities. One approach to improve the performance of carbon anodes is edge‐nitrogen doping, which effectively enhances the K‐ion adsorption energy. It remains challenging to achieve high edge‐nitrogen doping due to the difficulty in controlling the nitrogen dopant configuration. Herein, a new synthesis strategy is proposed to prepare carbon anodes with ultrahigh edge‐nitrogen doping for high‐performance PIBs. Specifically, self‐assembled supermolecule precursors derived from pyromellitic acid and melamine are directly pyrolyzed. During the pyrolysis process, the amidation and imidization reactions between pyromellitic acid and melamine before carbonization enable the successful carbonization of pyromellitic acid–melamine supermolecule. The obtained 3D nitrogen‐doped turbostratic carbon (3D‐NTC) possesses a …