Novel binderless carbon nanotube aerogel (CNAG) electrodes are developed. The materials exhibit a remarkable specific surface area of 1059 m(2) g(-1) with a special textural porosity with almost equal amounts of mesopores and micropores. These nanostructured CNAG electrodes (see figure) have a wide range of potential applications in electrochemical power sources. The CNAGs great potential as electrodes for supercapacitor applications is demonstrated by a specific capacitance as high as 524 F g-1.