Highly ordered mesoporous silica, Santa Barbara Amorphous-15 (SBA-15), and titanium-substituted mesoporous silica (TiSBA-15) materials were successfully synthesized, characterized, and evaluated. The textual and structural properties of the prepared materials with various titanium contents were characterized by inductively coupled plasma-mass spectrometer (ICP-MS), powder X-ray diffraction (XRD) patterns, nitrogen physisorption isotherms, scanning electron microscopy (SEM), and transmission electron microscopy (TEM). A limited content of titanium could be effectively substituted into the framework of SBA-15 without provoking structure change. The adsorptive performance was examined by methylene blue (MB) adsorbed on prepared materials. The isotherm models were analyzed to describe the adsorption behavior of prepared materials. The adsorption isotherms were well-fitted with Langmuir and Freundlich models in the simulation of the adsorption behavior of dyes. The SBA-15 and TiSBA-15 materials were found to be effective adsorbents for MB from aqueous solutions. The photodegradation of MB and total organic carbon (TOC) analysis on solid composites were used to evaluate the catalytical performance of Ti-containing mesoporous silica. The synergistic effect of adsorptive and photocatalytical ability of prepared TiSBA-15 was identified. The regeneration and cyclic performance were also proved. These results revealed that TiSBA-15 could be one effective alternative material for dye removal.