The structure−property relationships of nanostructured Ru/carbon aerogel composite materials havebeen evaluated. These new materials were prepared via a novel two-step metal vapor impregnation methodwhich enables one to control the Ru loading through repetition of the process. The resulting microstructureis characterized by highly dispersed Ru particles (≈20−30 Å in diameter) attached to the carbon aerogelsurface and distributed homogeneously throughout the material; the open pore structure of the carbonaerogels remains largely unaffected. Electrochemical characterization indicates that it is possible to increasethe specific capacitance of the carbon aerogels in 1.0 M H2SO4 from ≈100 F/g to greater than 250 F/g forsamples with >50 wt % Ru due to the pseudocapacitive properties of hydrous RuO2. A volumetric capacitancegreater than 140 F/cm3 was observed for some samples. In addition, these materials show good cyclingcharacteristics. Electrochemical impedance spectroscopy was unable to distinguish between double-layercapacitance and pseudocapacitance in these materials.