Catalytically grown graphite nanofibers (GNF) are molecularly engineered structures that are produced by the interaction of carbon-containing gases with small metal particles at temperatures around 600 degrees C. The fibrous solids consist of minuscule graphene sheets stacked at various angles with respect to the fiber axis. This arrangement generates a material possessing unique chemical properties because unlike conventional graphite crystals, only edges are exposed. Such a conformation produces a material composed entirely of nanopores that can accommodate small-sized adsorbate molecules, such as hydrogen, in the most efficient manner. In addition, the nonrigid pore walls can expand to accommodate the gas in a multilayer conformation. GNF exhibit extraordinary behavior toward the sorption and retention of hydrogen at high pressures and abnormally high temperatures. In this paper we discuss some of the critical factors involved in the adsorption of molecular hydrogen and the influence that this process exerts on the structural characteristics of the material. In addition, the deleterious effect of water vapor on the performance of the GNF is highlighted.