The capacities of hydrogen storage at room temperature under moderate presure amounted to 0.9 and 0.4 wt %, for periodic mesoporous organic-and inorganic-silica materials, respectively.Hydrogen has received much interest as an energy source for the replacement of fossil fuels in fuel-cell vehicles and portable electronics due to its clean combustion and high heating value. The development of fuel-cell vehicles and portable electronics will require new materials that can store large amounts of hydrogen at ambient temperature and relatively low pressures while possessing a small volume, low weight, and fast kinetics for recharging.1 However, no practical means for hydrogen storage and transportation have yet been developed. 2 Various materials including metal hydride, chemical hydride, carbon nanostructures, and metal-organic frameworks (MOFs) have been employed for hydrogen storage. 3 This area has been dominated by announcements of high-storage capacities in carbon nanostructures over the past few years. 4 However, a critical review shows that at room temperature and moderate pressure carbon nanostructures cannot store the amount of hydrogen required for automotive applications.5 Recently, MOFs have received much attention as a new approach for preparing porous materials because it allows more flexible and rational design of such materials. 6 However, a serious shortcoming of these materials has been the framework's instability, such as the collapse of the framework upon guest molecule removal.One candidate for a hydrogen-storage medium is based on a certain type of periodic mesoporous organic-silica material that appears to have the potential to store hydrogen under conditions of room temperature and moderate pressure.3,7 These materials possess the high surface area and porosity of carbon nanotubes and MOFs that may be important for adsorption of hydrogen. In view of their excellent properties, we chose to examine the porosity and hydrogen-storage properties of the mesoporous organic-silica (benzene-silica) material. We have also examined the hydrogen-adsorption capacities of the mesoporous inorganic-silica material in the absence of the benzene moieties, which play an important role in hydrogen uptake, as a comparison. Herein, we first report the adsorption of hydrogen at 78 K and room temperature under moderate pressure by the novel periodic mesoporous organic-and inorganic-silica materials with ordered open channels.The mesoporous organic-silica material was synthesized as described previously. 8 The synthesis of the mesoporous inorganic-silica material was similarly performed following the procedure of Stucky and co-workers, as detailed in the Electronic Supporting Information. 9 Figure 1 shows TEM images of periodic mesoporous organic-and inorganic-silica materials employed for hydrogen storage and clearly shows the formation of ordered mesostructures with a hexagonal arrangement of mesoporous channels. In the powder X-ray diffraction (PXRD) patterns (Supporting Information), the low-angle X-ray diffrac...