rapid charging characteristics, long cyclic life, and high power density. [5][6][7] However, the relatively low energy density of the supercapacitors is still the main obstacle to their wide range of commercial applications. [8][9][10] Consequently, how to enhance the energy density of carbon-based supercapacitors without sacrificing power density has attracted considerable attention.The specific capacitance and rate capability of supercapacitors, or more intuitively, the number of adsorbed charges and the rate of electron transfer, are mainly controlled by the electrode materials. [11][12][13] To achieve excellent electrochemical performance, the desirable carbon electrode materials of the supercapacitors should possess large specific surface area (SSA), adjustable pore structure/rational hierarchical porosity, and outstanding interface activity, so that it can achieve more efficient absorption, transfer and infiltration of the electrolyte ion. [14][15][16][17][18] Since the smaller pore size of the electrode material is conducive to the higher SSA, massive micropores and mesopores should be introduced to the electrode materials, in order to provide abundant adsorbed sites for charged ions. [19,20] However, the markedly reduced pore size will result in the impermeability of electrolyte ions among the near-confined pores, thus significantly decrease the electrochemical performance. Hence, the optimization of the pore structure and the regulation of the pore distribution are key strategies to improve the device performance.Heteroatom doping of carbon materials can also greatly impact the electrochemical performance of the supercapacitors. [21][22][23] On one hand, the heteroatoms including oxygen (O), nitrogen (N), sulfur (S), and phosphorus (P) elements can increase the total capacitance of supercapacitors by inducing pseudocapacitance in Faradaic redox processes. On the other hand, the decoration of O/N/S functional groups on the surface of the microporous and mesoporous carbon materials can considerably accelerate the migration of aqueous electrolyte ions by decreasing the migration resistance. [5,8] Thus, in order to fabricate high-performance supercapacitors, it is extremely necessary to design a kind of electrode materials with adjustable pore structure, rational hierarchical porosity, and appropriate heteroatom doping. Despite that the pore engineering and elemental doping have been demonstratedThe porous structure and heteroatom doping are crucial for the electrochemical performance of carbon materials for supercapacitors. However, designing carbon materials with appropriate pore sizes and heteroatom content is still facing daunting challenges. Herein, simultaneous regulation of porous structure and heteroatom doping in superabsorbent resin (SAR)-based activated carbon aerogels (SACAs) is implemented by facilely immersing superabsorbent resin in methylene blue (MB) solution with different concentrations, and then followed by freeze-drying and carbonization. The resulting SACAs possess variable oxygen/nitro...