Hydrophobic functionalized SBA-15 has been developed via postsynthesis modification with trimethylchlorosilane (TMCS) and used for volatile organic compounds (VOCs) removal. The adsorption and desorption performance of different SBA-15-TMCS under static and dynamic conditions were investigated. Experimental results indicated that all samples showed a highly ordered two dimensional hexagonal mesostructure, and the organic groups were chemically incorporated into the pore surface of SBA-15 substrate. Comparing with commercial silica gel and activated carbon, SBA-15-TMCS shows higher static adsorption capacities of n-hexane and 93# gasoline, good recyclability, lower water vapor adsorption capacity, higher dynamic adsorption capacity, and longer breakthrough time. The high adsorption efficiency and stability of SBA-15-TMCS are associated with their hydrophobic surface, uniform and large pore size, high surface area and pore volume. The designed SBA-15-TMCS with high VOC adsorption capacity and recyclability shows great potential for VOC removal.