Zinc-ion hybrid capacitors (ZHCs) represent a promising class of energy storage devices. However, the rational design of cathode materials rich in active sites for efficient Zn2+ storage remains challenging. Through a hierarchical modulation strategy designed to synergistically optimize the pore structure and surface chemistry of carbon material, we develop a N/P/O co-doped, coal tar pitch (CTP)-derived hierarchically porous carbon (NP-OPC) for effectively zinc storage. Acid oxidation effectively suppresses polycondensation of CTP, while pre-carbonization with N/P dopant generates an initial porous framework in the carbon precursor and a heteroatom-affine environment, collectively enhancing the efficiency of KOH activation and promoting heteroatom doping during carbonization. The resulting NP-OPC possesses a well-developed hierarchical porosity, an ultrahigh surface area of 3522.2 m2 g−1, and substantial heteroatom doping of N (∼6.12 at.%), P (∼2.07 at.%), and O (∼8.14 at.%). The structural properties provide sufficient active sites for Zn2+ adsorption, rapid ion/electron transport, and optimized surface physicochemical properties. Consequently, the NP-OPC based aqueous ZHC delivers an exceptional capacity of 207.3 mAh g−1 at 0.2 A g−1 and exhibits exceptional cycling stability, retaining 91.1% of its initial capacity after 30,000 cycles at 10 A g−1. Moreover, the assembled pouch device achieves both high energy density (138.6 Wh kg−1) and superior durability (89.5% capacity retention after 70,000 cycles at 10 A g−1). Through ex situ analyses and theoretical calculations, we elucidate the charge storage mechanism and identify the origin of the enhanced performance. This study offers a new avenue for the design of high-performance carbon materials derived from CTP.
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