Catalytically grown graphite nanofibers (GNF) are molecularly engineered st
ructures that are produced by the interaction of carbon-containing gases wi
th 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 en
tirely of nanopores that can accommodate small-sized adsorbate molecules, s
uch as hydrogen, in the most efficient manner. In addition, the nonrigid po
re walls can expand to accommodate the gas in a multilayer conformation. GN
F exhibit extraordinary behavior toward the sorption and retention of hydro
gen at high pressures and abnormally high temperatures. In this paper we di
scuss some of the critical factors involved in the adsorption of molecular
hydrogen and the influence that this process exerts on the structural chara
cteristics of the material. In addition, the deleterious effect of water va
por on the performance of the GNF is highlighted.