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The efficient storage of strategic gases—CH₄, CO₂, and H₂—remains a critical challenge due to the need for high pressures or cryogenic temperatures to achieve sufficient storage densities, often resulting in energy- and cost-intensive processes. Adsorption-based storage using porous materials offers a promising alternative. In particular, ordered mesoporous carbons, such as CMK-8 and CMK-9, are attractive due to their mechanical, thermal, and chemical stability, as well as their highly tunable textural properties. Surface functionalization can further enhance gas uptake, though the effect is often gas-specific. This study investigates the adsorption performance of four carbon materials: pristine CMK-8 and CMK-9, and their oxygen-functionalized counterparts produced via HNO₃ treatment. The adsorption capacities for CH₄, CO₂, and H₂ were evaluated through a combination of experimental gas adsorption measurements and molecular simulations. The results reveal structure–property relationships between surface chemistry and gas-specific adsorption behavior, with implications for the rational design of carbon-based materials for gas storage.