Advancement in the efficient energy storage is essential to keep up with the increasing demands in powering portable electronic gadgets and electric automobiles. [1,2] Carbon-based electrodes used in supercapacitors have remained fascinating means for efficient and environment-friendly electrochemical energy storage because of their Earth abundance, low cost, high specific surface area, and availability in easily tunable architectures and chemical states. [2,3] As compared with a pseudocapacitor where the charge is stored through fast Faradaic redox reactions, the electric double-layer capacitor (EDLC) stores charge at the interfaces through charge transfer between the electrolyte and the electrodes and, hence, provides faster charge-discharge cycling and specific capacitance of few orders of magnitude higher. [2] In the last decade, numerous carbon-based materials in various architectures have been utilized in EDLCs to achieve higher specific capacitance by increasing the specific surface area, crystallinity, conductivity, and density of electrochemically active sites. [1][2][3][4] Ideally, the well crystalline carbon-based allotropic nanomaterials, such as graphene, carbon nanotubes, and their hybrids in different 3D architectures, have so far been well studied for energy applications. [2][3][4][5] It has been recently observed that structural defects and heteroatom(s) doping into graphitic carbon lattices enhance their energy storage capability. [2,4] A clear conclusion on the best heteroatom(s), the atomic configuration of the dopant(s), and/or the defect-type in a graphitic carbon lattice for energy storage has not yet been achieved, because the related parameters are exclusively interdependent.In a complete contrast, very recently, the amorphous carbon-based materials have been reported to demonstrate attractive energy storage and conversion applications, such as in electrochemical batteries with high storage capacity and long-term stability, primarily owing to their disordered and defect-rich structures. [6][7][8][9][10][11][12][13][14][15] As such, it has been reported that the N-doped amorphous carbon sphere is more active for oxygen reduction reaction in 0.5 M H 2 SO 4 medium than their graphitic counterparts due to the fact that the micropores in amorphous carbon phase close down during graphitization process along with the decrease in N content. [14] Honda et al. reported that the disordered sp 2 clusters in amorphous carbon or a mixed carbon state (sp 2 þ sp 3 C matrix) are more beneficial to electrocatalytic activities than pure graphitic carbons due to abundance in trapped charged centers. [13] Recently, CoO/Co-amorphous