Homogeneous mesoporous zirconium-containing MCM-41 type silica were prepared by supramolecular templating and their textural and structural properties were studied using powder X-ray diffraction, N2 porosimetry, atomic force microscopy, EXAFS, XPS, and UV–VIS–NIR diffuse reflectance spectroscopy. Their acid properties were also studied by using IR spectroscopy and by the use of catalytic tests such as the decomposition of isopropanol and the isomerization of 1-butene. The materials prepared show a good degree of crystallinity with a regular ordering of the pores into a hexagonal arrangement and high thermal stability. The specific surface area of the prepared materials decreases as the zirconium content rises. Zirconium atoms are in coordination 7 to 8 and located at the surface of the pores such that a high proportion of the oxygen atoms bonded to zirconium corresponds to surface non-condensed oxygen atoms. Both facts are responsible for the acid properties of the solids that show weak Brønsted and medium strong Lewis acidity.