Theoretical (thermodynamic) and experimental backgrounds are considered for developing a much simpler, more technological and effective method (in comparison with the known megabar compression dynamic and static methods) of producing a high-density solid molecular ("reversible") hydrogen carrier by means of hydrogen intercalation (at the cost of the hydrogen association energy) in carbonaceous nanomaterials (between graphane-like layers) at relevant temperatures and pressures. As is shown, one of the processes of chemisorption of hydrogen in carbonaceous nanomaterials may be related to formation of graphane-like (carbohydride-like) complexes and/or multilayer graphane-like nanostructures. In this connection, some aspects of the graphene/graphane problem are considered, as well. By using gravimetric and electron microscopy data, the density values ( H = 0.7±0.2 g(H 2 )/ 3 (H 2 ), and * H = 0.28±0.08 g(H 2 )/ 3 (system) -the "volumetric" capacity) of the intercalated solid molecular ("reversible") hydrogen (of a high purity) in graphane-like nanofibers ( 15 mass % H 2 -the "gravimetric" capacity) have been defined. It is a much more acceptable, safe and efficient technology, in comparison with the current technologies of composite vessels with high hydrogen pressure (about 80 MPa) and the current space cryogenic technologies of hydrogen on-board storage in fuel-cell-powered vehicles. It exceeds and/or corresponds to the known U.S. DOE requirements-targets for 2015, with respect to the hydrogen capacities, safety, reversibility and puirity.Keywords: Carbon-based nanomaterials, High-density solid molecular reversible hydrogen carrier, Graphane-like (carbohydride) multilayer nanostructures, Graphene/graphane problem, Hydrogen on-board efficient and safety storage.