The one-dimensional channel array of hexagonal tungsten bronze (WO3) offers an electron transfer matrix, but its overwhelming H+ adsorption hinders it from being a good supercapacitor electrode material. Inspired by the Volcano plot on the relation between transition-metal and free energy of H-adsorption, we propose a new strategy to anchor transition metal ions (Zn2+, Cu2+, Ni2+, Ag+, Au3+ and Ir3+) into the WO3 lattice to improve proton-insertion based pseudocapacitance. Among the variety of transition metals, Zn2+ exhibits the optimal O 2p band center, which matches well with the best experimental capacitive behavior. The molar ratio of Zn/WO3 ranges from 0.2 to 0.6. The specific capacitance for Zn2+-anchored WO3 (390 F g-1) reaches 202% of that of WO3 (193 F g-1) at 0.5 A g-1 with robust stability (259 F g-1 at 3 A g-1 for 3000 cycles). Density functional theory confirms that O 2p is shifted down by the d-filling cations, which corresponds to alleviated O-H interaction and facilitated H+ desorption. The band tuning by transition-metal-ion incorporation would break new ground on developing high-capacitance metal oxide supercapacitors.