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A major advantage of highly crosslinked, organic aerogels is the ability to transform many of these materials into electrically conductive carbon aerogels. Carbon aerogels have been formed as monoliths, microspheres, irregularly-shaped powders, and thin film composites. In all cases, the carbon aerogels retain their high surface area (400–800 m²/g) and ultrafine cell/pore size (<100 nm). Carbon aerogels are being examined as electrodes for double layer capacitors, pseudocapacitors, and capacitive deionization units. This paper examines the synthesis, structure–property relationships, and performance of carbon aerogel electrodes used in electrochemical applications.