etc.), SCs, as a compelling green energy device, have attracted considerable attention due to their long cycle life, low cost, fast charge/discharge efficiency, and high power density. [6] SCs can be divided into electrical double layer capacitors (EDLCs) and pseudocapacitance capacitors based on different charges storage mechanisms. [7] EDLCs are based on electrostatic adsorption of electrolyte ions at the double layer interface formed between electrolyte and electrode to store charge, [8] whereas the pseudocapacitance capacitors store energy through Faradaic redox reactions of metal compounds (e.g., MnO 2 , MoS 2 , Ni(OH) 2 , etc.), [9] conducting polymers (polypyrrole, polyaniline, and polythiophene), or heteroatoms (N, O, B, S, etc.). [10] However, SCs have been criticized for its low energy density at larger power density and poor capacitance under high current density in practical applications, which limit further applications. [11] Therefore, it is important to explore new functional electrode materials with ideal performances for nextgeneration EES. [12] As key components of SCs, the electrode active materials determine the total electrochemical performance for SCs. [13] Carbon materials, including activated carbons, carbon nanotubes, graphene, and carbon spheres, are considered to be ideal electrode materials due to their environmental friendliness, low cost, availability, and open porous structure. [14] As an ideal EDLCs electrode materials, [15] the hierarchical microand mesopores carbon spheres possess the following advantages: i) The three dimensional (3D) spheres architecture has larger specific surface area (S BET ) and higher electrical conductivity. [16] ii) The well-dispersed porous carbon spheres facilitated electrolyte infiltration and accelerated ions transport in the electrolyte. [17] iii) The outstanding structure stability ensures that the electrode material will not be structurally damaged at high current density. [18] Although pure carbon materials could obtain favorable performance stability and structural durability in electrochemical work, it cannot satisfy the further improvement of capacitance. [19] Therefore, the doping of heteroatoms in the carbonaceous materials introduces pseudocapacitance besides EDLCs, [20] which can further effectively The N/O co-doped hierarchical porous graphitized carbon microspheres (N/O-PCs) are successfully prepared by condensation polymerization of 5-hydroxymethylfurfural and melamine, and subsequent KOH activation strategy. The obtained carbon materials have a high specific surface area (1685.58 m 2 g -1 ), rich micro-and mesopores, and appropriate pore volume (0.828 cm 3 g -1 ). The degree of graphitization for N/O-PCs is improved because the ratio of I G and I D increases from 0.88 to 1.03. The layer spacing of the lattice plane (002) for the N/O-PCs is enlarged, facilitating the transmission of electrolyte ions. The high graphitization degree and enlarged layer spacing bring excellent electrical conductivity and wettability for N/O-PCs as...