In principle, supercapacitors may store electrical energy through the electrical double-layer capacitance (EDLC), pseudocapacitance, or a mix of the above two. [3f ] EDLC stems from the electrostatically reversible electrolyte ion adsorption and desorption on electrode surfaces. [4] Therefore, electrodes with a large specific surface area and good electrical conductivity are essential to obtain a high EDLC. Carbon materials, such as activated carbon, [5] graphene, [6] and carbon nanotubes (CNTs), [7] are common EDLC materials due to their large specific surface area, high electrical conductivity, good cycling stability, and reasonably low cost. On the other hand, pseudocapacitance originates from rapid and reversible Faradaic reactions occurring on the surfaces of redox-active electrodes. [8] Common pseudocapacitive materials include transition metal oxides and conducting polymers. [9] Further, asymmetric hybrid capacitors combine electrodes with EDLC and pseudocapacitance to obtain broader operating potential windows and substantially higher energy density. [10] The properties of capacitive electrode materials govern the energy storage performance of supercapacitors. Extensive research efforts have been devoted to developing novel capacitive materials. These efforts have focused on two main strategies: 1) increasing the ion-accessible surface area of capacitive materials and 2) incorporating redox-active species to increase pseudocapacitance, achieving significant progress. For instance, a 3D graphene framework prepared by thermal decomposition exhibited a large specific surface area of 1018 m 2 g −1 and a high specific capacitance of 266 F g −1 at a current density of 0.5 A g −1 . [11] A nanoporous carbon sphere with an exceptional specific surface area of 3357 m 2 g −1 showed a specific capacitance of 405 F g −1 at 0.5 A g −1 . [12] Many studies have optimized the crystallinity, pore structure, and redox-active species of metal oxides/hydroxides and polymeric materials. [13] However, irregular pore structures, low electrical conductivity, uneven distribution of redox-active species in capacitive materials, and uncontrollable agglomeration of their nanoparticles often increase the mass transfer resistance of electrolyte ions and reduce their accessible surface areas, resulting in deteriorated energy storage performance. Further, metal dissolution and crystal structure transformation of metal oxides/hydroxides and fast degradation of polymeric materials also shorten the cycling life of supercapacitors fabricated using these materials. [14] Therefore, developing novel capacitive materials with Covalent-organic frameworks (COFs) are emerging organic crystalline materials with a porous framework that extends into two or three dimensions. Originating from their versatile and rigorous synthesis conditions, COFs have abundant and tunable pores, large and easily accessible surfaces, and plenty of redox-active sites, making them promising material candidates for various energy storage applications. One important area...