Phloroglucinol-Formaldehyde (PF) organic aerogels were prepared from alcoholic sol-gel polycondensation of phloroglucinol with formaldehyde using KOH as base catalyst and followed by supercritical drying with carbon dioxide. Subsequent pyrolysis of PF organic aerogel under He flow produced carbon aerogels. Textural properties of PF organic and carbon aerogels were obtained by nitrogen adsorption-desorption, and their specific capacitances were measured by cyclic voltammetry. The resultant PF carbon aerogels were mostly mesoporous material with high surface area. The nanoporous structure and electrochemical behavior of PF carbon aerogels could be controlled by the molar ratio of phloroglucinol to catalyst (P/C) and carbonization conditions. PF carbon aerogels exhibited the highest surface area in excess of 1,200 m2/g and specific capacitance up to 250 F/g in comparison to other carbons.