Efficient hydrogen storage is essential for its use as a sustainable energy carrier. Diatomaceous earth, a high-surface-area siliceous geomaterial, shows potential as a physisorption material for hydrogen storage. This study analyzes diatomaceous earth's long-term characteristics when subjected to high-pressure hydrogen injection. The diatomaceous earth was subjected to a hydrogen pressure of 1200 psi for a period of 80 days at room temperature. Neither notable morphological or mineralogical changes were observed. Nevertheless, there was a slight reduction in fine particles and a slight increase in larger particles. The Brunauer−Emmett− Teller (BET) surface area decreased slightly with a significant decrease in pore width. However, the hydrogen adsorption at 77 K temperature was increased significantly (45.5%) after the hydrogen storage test. Moreover, there was a delayed release of molecular water as the temperature increased. These changes suggest that a condensation reaction has occurred involving some of the opal-A silanol groups (Si−O−H), producing molecular water. Bonding through siloxane bridges (Si−O−Si) results in a significant decrease in pore width and increased hydrophobicity (i.e., the interaction between diatomaceous surface and H 2 was increased), thereby enhancing hydrogen adsorption capacity. These findings indicate that diatomaceous earth holds promise as a material for hydrogen storage, with the potential for its hydrogen adsorption capacity to improve over time.