<p>This work presents a rational design of oxygen-functionalized hierarchically porous carbon sheets for high-performance zinc-ion hybrid supercapacitors (ZHSs) via a dual-role activation strategy, simultaneously micropores and introducing oxygen dopants. Using anthracene as a carbon precursor and KCl as a structural template, the optimized electrode achieves exceptional electrochemical performances with a specific capacity of 134.3 mAh g⁻¹ (0.05 A g⁻¹) and an energy density of 101.5 Wh kg⁻¹ (34 W kg−⁻¹) in 3&#xa0;mol L⁻¹ ZnSO₄ electrolyte. Remarkably, employing a 3&#xa0;mol L⁻¹ Zn(CF₃SO₃)₂ electrolyte further enhances the capacity to 142.4 mAh g⁻¹ (0.05 A g⁻¹) and energy density to 127.9 Wh kg⁻¹ (23 W kg⁻¹), while achieving outstanding cycling stability (74.8% retention after 50,000 cycles at 5 A g⁻¹). Mechanistic studies unveil a synergistic charge storage mechanism in Zn(CF₃SO₃)₂⁻&#xa0;based systems, combining electric double-layer capacitive behavior via CF₃SO₃−&#xa0;anion adsorption and diffusion-controlled Zn²⁺ redox intercalation. This work proposes a material-electrolyte co-engineering strategy, elucidating the synergistic effects of oxygen-functionalized carbon surfaces, tailored pore hierarchy, and anion chemistry in enabling high-energy and long cycle ZHSs for practical energy storage.</p>