Magnesium-based hydrogen-storage materials were prepared by reactive ball-milling under hydrogen atmosphere. It was shown that crystallitic carbon from anthracite carbonization was an effective milling aid for magnesium. Dispersive nano-particles about 20 to 60 nm were prepared from magnesium with 35 wt.% of crystallitic carbon additive by milling for 3 h under 1 MPa of hy-drogen atmosphere. The magnesium hydrided into MgH2 and the crystallitic carbon was endowed with C=CH2 functional group during milling. The hydrogen-storage materials were used for the hy-drodesulfurization of CS2 and thiophene, and H2S and MgS yielded after reaction. To add molybdenum into the hydrogen-storage materials was in favor of the hydrogenation of sulfo-compounds.