This study presents carbon aerogels derived from anion-modified nanocellulose for adaptive supercapacitor performance. The research explores how anion selection influences the electrochemical properties of carbon aerogels (CAs) through cation-induced cross-linking of cellulose nanocrystals (CNCs). The study highlights the critical role of residual anions in modulating the physicochemical properties of CAs, which in turn affects the performance of supercapacitors. The use of anion-modified nanocellulose enables the creation of CAs with tailored porosity and surface area, enhancing their electrochemical performance. The study also introduces the concept of electro-assisted (EA) wetting, which improves electrode wettability and electrolyte infiltration, leading to enhanced charge storage and overall performance. The results show that CA-Nit, derived from calcium nitrate, exhibits the highest specific capacitance and energy density, demonstrating the effectiveness of anion modulation in optimizing supercapacitor performance. The study also evaluates the cycling stability of CA-Nit, showing that it retains high capacitance even after 10,000 charge-discharge cycles. The findings emphasize the importance of wettability in electrochemical performance and suggest that current supercapacitor materials may only be utilizing a fraction of their potential due to suboptimal wettability. The research contributes to the development of more efficient and sustainable supercapacitors using earth-abundant materials.This study presents carbon aerogels derived from anion-modified nanocellulose for adaptive supercapacitor performance. The research explores how anion selection influences the electrochemical properties of carbon aerogels (CAs) through cation-induced cross-linking of cellulose nanocrystals (CNCs). The study highlights the critical role of residual anions in modulating the physicochemical properties of CAs, which in turn affects the performance of supercapacitors. The use of anion-modified nanocellulose enables the creation of CAs with tailored porosity and surface area, enhancing their electrochemical performance. The study also introduces the concept of electro-assisted (EA) wetting, which improves electrode wettability and electrolyte infiltration, leading to enhanced charge storage and overall performance. The results show that CA-Nit, derived from calcium nitrate, exhibits the highest specific capacitance and energy density, demonstrating the effectiveness of anion modulation in optimizing supercapacitor performance. The study also evaluates the cycling stability of CA-Nit, showing that it retains high capacitance even after 10,000 charge-discharge cycles. The findings emphasize the importance of wettability in electrochemical performance and suggest that current supercapacitor materials may only be utilizing a fraction of their potential due to suboptimal wettability. The research contributes to the development of more efficient and sustainable supercapacitors using earth-abundant materials.