Atomic hydrogen storage by carbon nanotubes (CNTs) and highly oriented pyrolytic graphite (HOPG) has been studied using a flow catalytic reactor and an ultra-high vacuum surface science apparatus including scanning tunneling microscope (STM), respectively. Defect sites on CNTs as adsorption sites of atomic hydrogen are introduced by oxidation pretreatment using La catalyst. Pd catalysts are then deposited on CNT surfaces for dissociation of H 2 into atomic hydrogen, which spills over to the defect sites. In the best case, 1.5 wt% of hydrogen is stored in the defective CNT with Pd particles at 1 atm and 573 K. In temperature programmed desorption (TPD) experiments, H 2 starts to desorb at 700-900 K depending on the annealing temperatures of CNTs prior to hydrogen storage. On the HOPG surface, hot atomic hydrogen produced by dissociation of H 2 using tungsten wire desorbs from graphite terraces at 400-700 K, which is much lower than that on CNTs. It is possible that one can decrease the desorption temperature by changing the method of H 2 dissociation. q