A key technology for natural gas vehicles is the removal of H2S trace content from fuel. In previous studies, purification based on the adsorption principle has been proved to have low separation cost, and the selection of an adsorbent is a crucial factor in this method. To enhance H2S sorption capacity, an ordered SBA-15 silica mesoporous material with a high specific surface area is synthesized as a carrier of triethanolamine (TEA). The mesoporous molecular sieve SBA-15 coated with a TEA film considerably enhances H2S sorption capacity. The effects of operational variables on H2S removal efficiency, including the amount of TEA-loading, adsorption pressure, flow rate, and fixed bed length, are investigated with a single-column adsorption apparatus. A model demonstrating H2S dynamic sorption processes through as TEA-modified adsorbent bed is proposed. The model fits well the experimental data and can be applied to the H2S sorption process simulation and optimal process design.