Titanium oxide species were loaded within the framework of mesoporous materials (Ti-HMS) by hydrothermal synthesis. These Ti-HMS exhibited high and unique photocatalytic reactivity for the decomposition of NO into N-2 and O-2 at 275 K. In situ diffuse reflectance absorption and XRD investigations indicated that the titanium oxide species were dispersed well within the zeolite framework and isolated in tetrahedral coordination with low Ti content.