This study focusses on obtaining heterogeneous Ti-containing catalysts through the designrnand optimization of pure silica SBA-15 and hybrid organic-inorganic PMO mesostructuredrnmaterials in which the pore size, the particle morphology, and the surface chemistry arerncontrolled to enhance the accessibility of the active sites and to avoid diffusion problemsrnof substrates and products. The synthesis conditions of pure silica SBA-15 and hybridrnorganosilica PMO materials with different particle morphologies and pore sizes have beenrnoptimized. Ti has been incorporated in the framework/on the channel of both types ofrnordered mesoporous materials by using either co-condensation or grafting methods. To dornthis, the optimum SBA-15 and PMO materials, which have different pore diameters havernbeen selected for Ti-grafting. A strategy has been designed to incorporate Ti in thernframework of the mesoporous material during the support synthesis step (cocondensation).rnA detailed study has been undertaken to analyze the use of differentrnsurfactants, different Ti-source precursors, additives and different Ti/Si ratios of thernsynthesis gel to obtain Ti-incorporation in the Td structure and thereby avoiding orrnminimizing the agglomeration of TiO2 species. The prepared samples were characterizedrnby X-ray diffraction (XRD), Thermogravimetric Analysis (TGA), N2 adsorptiondesorptionrnisotherms, Scanning Electron Microscopy (SEM), Transmission ElectronrnMicroscopy (TEM), Inductively Coupled Plasma Optical Emission Spectroscopy (ICPivrnOES) and Diffuse Reflectance UV-vis Spectroscopy (DRS UV-vis). The following TicontainingrnSBA-15 and PMO with different particle morphologies and pore sizes withrnisolated Ti (IV) species have been synthesized:rn- Ti-containing SBA-15 and PMO materials with hexagonal plate-like and fiber-likernparticle morphology using Pluronic P104 and P123 surfactants;rn- Ti-containing SBA-15 materials with hexagonal pore structure and large porerndiameters (> 10 nm) using TIPB micelle expander;rn- Ti-containing PMO materials with moderately ordered hexagonal pore structurernand large pore diameters (> 8.5 nm) using TIPB micelle expanders;rn- Ti-grafted SBA-15 and PMO materials with highly populated isolated Td Ti (IV)rnspecies and without formation of anatase TiO2 species.rnThe catalytic activities of selected catalysts were tested for the epoxidation of cyclohexenernusing TBHP (5.5 M in decane solution) as an oxidant. The catalysts which give goodrnconversion and epoxide selectivity in the epoxidation of cyclohexene were selected forrnepoxidation of vernonia oil. Solvent-free epoxidation of vernonia oil with anhydrous TBHPrn(5.5 M TBHP in decane solution) in the presence of selected Ti-containing SBA-15 andrnPMO catalysts was investigated. Ti-grafted materials show better catalytic activity thanrntheir corresponding Ti-containing materials, synthesized by the co-condensation method.rnTi-containing SBA-15 materials are better in conversion when compared to PMO type ofrnmaterials. Among them, Ti-grafted SBA-15 with large pore diameter (TiG-ESBA-L) givesrnthe highest conversion (71%) with 80% of epoxide selectivity. Ti-containing PMOrnmaterials are better in epoxide selectivity in epoxidation of vernonia oil (achieving morernthan 90% epoxide selectivity) when compared to their corresponding Ti-SBA-15 materials.