• B and N co-doped coal-based activated carbon achieves a high specific capacity of 371.4 mAh g−1 at 1 A g−1 for aqueous zinc-ion capacitors.
• The material retains 74% of its initial capacity after 10,000 cycles, demonstrating excellent cycling stability.
• Density functional theory calculations reveal that pyridinic N is crucial for enhancing Zn2+ storage and electrochemical reversibility.
• This work provides insights for designing high-capacity and ultrafast pseudocapacitive carbon cathodes for ZICs.
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