Abstract: A series of titanic-silica mesoporous materials have been synthesized by using the Gemini surfactant [C16H33(CH3)2N+(CH2)6N+(CH3)2C16H33]•2Br− (GEM16-6-16) as a template. The XRD patterns and TEM images provide the evidence that the mesoporous phases are changed according to the following path by varying the molar ratio of n(Ti)/n(Si): hexa nal mesoporous structures are obtained when n(Ti)/n(Si)≤0.20; cubic when n(Ti)/n(Si)=0.30; lamellar when n(Ti)/n(Si)=0.50; and amorphous when n(Ti)/n(Si)=1.0. The FT-IR spectra suggest that the amount of Ti—O—Si bonds in the framework increases with increasing n(Ti)/n(Si) initially, and reaches to a limit when n(Ti)/n(Si)≥0.20. Additionally, the ethanol and butanol have been approved that they can control the evolvement of silica mesoporous phase transition. Following that, the process of titanic-silica mesoporous phase transition has been elucidated by the aggregation of Ti—O—Si bonds and the effect of butanol produced from the hydrolysis of tetrabutyl titanate(TBOT).