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Aqueous Zn-ion hybrid supercapacitors (AZHSCs) combining the advantages of high‐energy batteries and high‐power supercapacitors see a bright future, but they still suffer from the poor capacity of carbonic cathodes. Herein, a functionalized porous carbon cloth (denoted as FPCC) electrode is demonstrated based on commercial carbon cloth (denoted as CC) tuning by structural and surface engineering. The constructed exfoliated porous carbon layer and the negatively charged functionalized interface not only increase the electrical double layer capacitance but also favor the chemical adsorption of Zn2+ to obtain additional pseudocapacitance. Consequently, the FPCC electrode delivers a high capacity of 0.16 mAh cm−2 at 4 mA cm−2, which is 923.8 times higher than CC, and a long cycle life (85.0% capacity retention after 30 000 cycles). More importantly, the Zn//FPCC AZHSC possesses an impressive energy density (3.3 mWh cm−3) and power density (240 mW cm−3), superior to many advanced batteries and supercapacitors. The quasi-solid-state device is also assembled as a demo. This modification strategy may provide new opportunities for high-performance AZHSCs. [ABSTRACT FROM AUTHOR]