This study investigates the impact of anion selection on the structural and electrochemical properties of carbon aerogels (CAs) derived from anion-modified nanocellulose for supercapacitor applications. The researchers used calcium acetate, calcium chloride, and calcium nitrate to cross-link cellulose nanocrystals (CNCs), forming aerogels with varying pore sizes and surface areas. The anion type significantly influenced the specific surface area (SSA) and pore size distribution, with calcium nitrate resulting in the highest SSA and smallest dominant pore size. Electrochemical tests, including cyclic voltammetry (CV) and galvanostatic charge-discharge (GCD) measurements, revealed that CA-Nit exhibited superior electrochemical performance, with a higher specific capacitance and energy density compared to other samples. The study also introduced electro-assisted (EA) wetting, which improved electrode wettability and further enhanced the electrochemical performance of CA-Nit. The EA wetting process led to a more uniform distribution of electrolyte within the narrow pores, improving ion diffusion and charge storage. The findings highlight the importance of anion selection and EA wetting in optimizing the performance of CAs for supercapacitor applications, providing a rational design approach to enhance the overall efficiency of these devices.This study investigates the impact of anion selection on the structural and electrochemical properties of carbon aerogels (CAs) derived from anion-modified nanocellulose for supercapacitor applications. The researchers used calcium acetate, calcium chloride, and calcium nitrate to cross-link cellulose nanocrystals (CNCs), forming aerogels with varying pore sizes and surface areas. The anion type significantly influenced the specific surface area (SSA) and pore size distribution, with calcium nitrate resulting in the highest SSA and smallest dominant pore size. Electrochemical tests, including cyclic voltammetry (CV) and galvanostatic charge-discharge (GCD) measurements, revealed that CA-Nit exhibited superior electrochemical performance, with a higher specific capacitance and energy density compared to other samples. The study also introduced electro-assisted (EA) wetting, which improved electrode wettability and further enhanced the electrochemical performance of CA-Nit. The EA wetting process led to a more uniform distribution of electrolyte within the narrow pores, improving ion diffusion and charge storage. The findings highlight the importance of anion selection and EA wetting in optimizing the performance of CAs for supercapacitor applications, providing a rational design approach to enhance the overall efficiency of these devices.