The hydrogen adsorption capacity of different types of carbon nanofibers (platelet, fishbone and ribbon) and amorphous carbon have been measured as a function of pressure and temperature. The results showed that the more graphitic carbon materials adsorbed less hydrogen than more amorphous materials. After a chemical activation process, the hydrogen storage capacities of the carbon materials increased markedly in comparison with the non-activated ones. BET surface area of amorphous carbon increased by a factor of 3.5 and the ultramicropore volume doubled, thus increasing the hydrogen adsorption by a factor of 2. However, BET surface area in platelet CNFs increased by a factor of 3 and the ultramicropore volume by a factor of 6, thus increasing the hydrogen storage by a factor of 4.5. The dependency of hydrogen storage capacity of carbon materials on the BET surface area was evaluated using both a condensation model and experimental results. Comparison of data suggests that the hydrogen adsorption capacity clearly depends on the pore structure and so, on the accessibility to the internal surface.