Supercapacitors employing electrochemical double layer capacitance (EDLC) for charge storage require electrode materials with high specific surface areas and narrow, nanoscale pore size distributions.[1,2] Activated carbons, which are cost-effective to produce and have the necessary surface area and pore geometries, are often used for this purpose.[2] Abundant biopolymers such as cellulose are interesting sources for activated carbon as their nanocrystalline forms can act as lyotropic liquid crystals in aqueous suspension, self-assembling into chiral nematic phases.[3] This helical structure can be maintained in aerogel materials,[4] permitting the construction of highly ordered scaffolds. In previous work, we exploited this behavior to develop porous hierarchically-ordered activated carbon aerogels from cellulose nanocrystals for use as supercapacitor electrodes.[5] While this work represented the first example of an activated carbon aerogel with chiral nematic CNC-derived hierarchical order, optimization of surface area and pore geometry was not performed. In this presentation, I will demonstrate our recent efforts to optimize the electrochemical performance of activated carbon aerogels. These materials may offer environmentally friendly energy storage solutions in the future.