Strategies followed to improve SBA-15 surface (essentially inert) included modifications by adding acidic or basic (or both) species during or after silica synthesis. Amphoteric properties are especially important, as some reactions (alcohol dehydration, for instance) require both types of sites to efficiently take place. In this work, single Zr (nominal 3, 5, and 10 wt%, as ZrOCl2•8H2O) direct addition during SBA-15 synthesis was used to impart amphoteric characteristics (as determined by NH3 and CO2 TPD) to mesostructured SiO2 matrices. Additional materials characterization included textural (N2 physisorption) and structural (XRD, FTIR, and UV–Vis spectroscopies, and HRTEM as well) studies. Actual solids composition was also determined (EDS). The degree of Zr incorporation into mesoporous silica was enhanced with nominal content in binary formulations, although not necessarily integrated into SBA-15 walls forming Zr-O-Si linkages. It seemed that single ZrO2 domains (framework and extra-framework) could provide suitable amphoteric properties by significantly increasing the number and strength of both acid and basic sites (especially formulations containing nominal 5 wt% Zr), as to those over mesostructured silica matrices. Also, potentially deleterious strong acid sites were avoided. The binary oxides present great potential to be applied in reactions requiring vicinal acid–base pairs (alcohol dehydration, for instance).