Mesoporous titanosilicates with 1-12 mol % Ti content and with three-dimensional wormhole-like mesoporosity are prepared by a modified sol-gel technique. Sorption analysis shows that there is little change in the surface properties with increasing Ti concentration in the samples, implying that Ti atoms either are well-dispersed on the walls of the silica matrix or are present inside the framework with no pore blocking effect. Spectroscopic analysis shows that the Ti atoms are atomically dispersed in the silica matrix even at very high Ti concentration and there is no observable Ti aggregate (anatase) present in the samples. These titanosilicate samples after ALL deposition followed by trimethylsitylation (for enhanced hydrophobicity) are highly efficient catalysts for vapor-phase propene epoxidation using O-2 and H-2. It was possible to achieve commercially desirable performance with about 7% propene conversion, >90% propene oxide selectivity, and about 40% hydrogen efficiency.