to their inherent merits of fast charge/ discharge rate, high power output, long cycle lifetimes, and lightweight. [3][4][5] However, the main bottleneck in the development of supercapacitors is to increase their energy density without sacrificing power density so that they can compete with rechargeable batteries. [6][7][8] Bimetallic copper-cobalt sulfide (CuCo 2 S 4 ) is a potentially promising battery-type electrode material for high energy storage applications, owing to their richer Faradaic redox reactions and better redox reversibility relative to corresponding mono-component sulfides and oxides. [9] Unfortunately, the reactivity kinetics of CuCo 2 S 4 is hindered by the slow ionic/electron transport. Up to now, extensive research on CuCo 2 S 4 nanostructures has been carried out, including hybridization with highly conductive skeletons to increase the exposed electrochemically active sites and nanostructuring to reduce the particle size. [10,11] Nevertheless, the electrochemical performance of these CuCo 2 S 4 -based nanostructures is still far below expectations, because these methods cannot fundamentally modulate their electrical properties while ion diffusion barriers have not been specifically addressed.Recently, anion defect engineering has been investigated to tune the electronic structure and the surface chemical properties of active materials. [12,13] This is because vacancies serving as donors can tune the charge density distribution to triggerThe ORCID identification number(s) for the author(s) of this article can be found under