Hydrogen trapping sites in hydrogenated nanostructured graphite (HNG) prepared by mechanical milling under hydrogen atmosphere were intensively studied with transmission electron microscopy (TEM) and electron energy-loss spectroscopy (EELS). Measurements ofand -plasmon dispersion and 1s ! 2p à excitation spectra of the graphitic matrix suggested the existence of at least two types of hydrogen trapping states: one was the conventional C-H covalent bond, and the other was related to the -orbitals of the carbon atoms extending normal to the graphene layers. We found that iron carbide particles incorporated as contamination during the mechanical milling also stored a significant amount of hydrogen, as revealed by the change in the Fe-L 2;3 spectrum when the sample was annealed. We re-assigned the assumed hydrogen trapping sites to the hydrogen desorption peaks in the thermal desorption spectrum (TDS) based on these experimental results.