A novel high-density hydrogen and other gas storage material has been fabricated and enhanced to provide the opportunity to use hydrogen as a predominant energy source by using hierarchical and ordered nanoporous materials to provide a solution to the shortcomings of current storage technologies. These materials consist of high aspect ratio porous templates with aligned and periodic nanocapillaries that have a tunable density, diameter, and wall thickness. Not only is the disclosed process low-cost and scalable, but catalytic fabrication of carbon nanotubes (CNTs) within the nanocapillaries is achieved, thereby yielding coaxial nanocapillary arrays for physical and adsorbed hydrogen storage with ultra-high gravimetric and volumetric hydrogen storage densities.