A new microporous TiO
2-pillared layered titanate has been prepared by hybridizing theexfoliated titanate with the anatase TiO
2 nanosol. The stable colloidal nano-sheet wasobtained by intercalating tetrabutylamine into the layered protonic titanate, H
xTi
2-x/4x/4O
4·H
2O(
x = 0.67), with a lepidocrocite-like structure. The colloidal suspension of exfoliated titanatesheets was mixed with the monodispersed anatase TiO
2 nanosol solution prepared by thehydrolysis of titanium isopropoxide with acetylacetone. The obtained nanohybrid was heatedat 300
C for 2 h in order to complete the grafting reaction of intercalated anatase TiO
2nanosol on the interlayer surface of layered titanate. According to the X-ray diffractionanalysis and N
2 adsorption-desorption isotherms, it was found that the TiO
2-pillared layeredtitanate showed a pillar height of ~2 nm, a high surface area of ~460 m
2/g, and a pore sizeof ~0.95 nm, indicating the formation of a microporous pillar structure. Its photocatalyticactivity was evaluated by measuring the total volume of H
2 gas evolved during the irradiationof the catalyst suspensions in water. The H
2 gas evolution was found to increase from thelayered titanate (cesium and protonic form) to the unsupported TiO
2 (acac-TiO
2) and theTiO
2-pillared layered titanate, because the electron and hole recombination in the pillaredsystem is thought to be effectively suppressed because of electron transfer between guestand host. A marked enhancement in the activity by ca. 40 times was obtained for TiO
2-pillared layered titanate compared to pristine compounds such as layered titanate andanatase TiO
2 nanosol when Pt (0.3 wt %) was doped on the surface of the sample.