Carbon nanostructures represent a revolution in science and hold the potential for a large range of applications because of their interesting electrical, mechanical, and optical properties. Multiwall carbon nanotubes and carbon nanofibers of herringbone formation were grown by chemical vapor deposition on different catalysts from a number of hydrocarbon sources. After the total or particle removal of the catalyst system, the carbon nanostructures were analyzed for hydrogen uptake. Six samples of nanofibers grown on a Pd-based catalyst system (with a surface area of 425-455 m(2)/g) were controlled oxidized in air, such that they had different ratios of Pd/C varying from 0.05 to 0.9 mole ratio. The hydrogen uptake experiments were performed volumetrically in a Sievert-type installation and showed that the quantity of desorbed hydrogen (for pressure intervals ranging from 1 to 100bars) by the carbon nanostructures free of any metal catalyst particles was between 0.04 and 0.33% by weight. For the samples of nanofibers that contained Pd in various Pd/C ratios, palladium revealed catalytic properties and supplied atomic hydrogen at the Pd/C interface by dissociating the H-2 molecules. The results show a direct correlation between the Pd/C ratio and the quantity of hydrogen absorbed by these samples. A saturation value of about 1.5wt.% was reached for a high ratio of about 1:1 of Pd/C. The multiwall carbon nanotubes grown on a Fe:Co:CaCO3 catalytic system and purified by acid cleaning and air oxidation showed a hydrogen uptake value of 0.1 to 0.2wt.%.