Hydrogen desorption and adsorption properties of the fullerene materials C60, C70, and fullerite (a mixture of C60 and C70) were measured volumetrically using a Sievert’s apparatus. Over several cycles of isotherm measurements at 77 K, the hydrogen storage capacities of one of the fullerite samples increased from an initial value of 0.4 wt % for the first cycle to a capacity of 4.4 wt % for the fourth cycle. Correspondingly, the surface area of this sample increased from 0.9 to 11 m2/g, and there were changes in its x-ray powder diffraction pattern. In comparison, two other fullerite samples, prepared by a different procedure showed no such behavior. Pure C60 and pure C70 were also cycled and exhibited small and constant capacities of 0.7 and 0.33 wt %, respectively, as a function of number of cycles. The enhanced storage capacity of fullerite material is tentatively attributed to the presence of C60 oxide.