In this work, we present the synthesis of Ag doped TiO2 materials. The products are characterized by powder X-ray diffraction, transmission electron microscopy, X-ray photoelectron spectroscopy, nitrogen adsorption, and hydrogen adsorption. The Ag/TiO2 materials exhibit 3.65 times higher in hydrogen adsorption capability compared with the non-doped TiO2 materials thank to the existence of Ti3+ species, which are Kubas-type hydrogen adsorption centers, and the Ag nanoparticles which provide spillover effects. We believe that this is the first time that both Kubas-type adsorption and spillover are exploited in the design of novel hydrogen storage materials.