Titanium-functionalized silica-pillared clays synthesized through post synthetic route was utilized as adsorbers for the removal of Cr(VI) ions from aqueous solutions under different temperatures and initial concentrations. The starting mesostructured silica-pillared clay is assembled by intragallery ammonia-catalyzed hydrolysis of tetraethoxysilane using cationic surfactant as gallery template, and subsequently, the formed interlayered pore walls were decorated with nano-sized TiO2 particle through organic titanium functionalization process. The kind of structural transformation has been confirmed by X-ray diffraction (XRD), nitrogen adsorption-desorption isotherms, Fourier transform infrared (FT-IR) analysis, UV-vis diffuse reflectance spectroscopy (DRS), elemental analysis (XRF), scanning electron microscopy (SEM) and transmission electron microscopy (TEM). Such results indicate that most of the grafted titanium species was combined with Si-OH on the surface of gallery pores. By changing the concentration of organic titanium source during synthesis, the porous structure system is effected. Under suitable conditions, these materials exhibit high adsorption capacity and efficiency. Qualitative estimates of the thermodynamic parameters showed that the overall adsorption process is spontaneous (Delta G degrees <0) and endothermic (Delta H degrees >0). The adsorption isotherms of Cr(VI) on titanium-functionalized silica-pillared clay were best fitted by Redlich-Peterson models. Detail results of thermodynamics and kinetics are also presented. (C) 2014 Elsevier B.V. All rights reserved.