Although previous researchers have found that FSM-16 (#16 Folded Sheet Mesoporous material) doped with chromium and related Cr-doped silica catalysts has shown great activity for the oxidative dehydrogenation of isobutane to isobutene, information on the nature of these catalysts is insufficient. For this study, three types of Cr-doped silica catalysts were prepared by applying the template ion exchange method. CrOx/FSM-16 and CrOx/SiO2 were used as references. These catalysts were used for oxidative dehydrogenation, which was then characterized via various techniques. The most active catalyst was Cr-doped silica, which did not have the hexagonal structure that is characteristic of mesoporous FSM-16. Various characterizations showed that the catalytic activity of the Cr-species, stemmed from a weak acidic nature and a redox nature that originated from the combination of silicate and a Cr cation, as opposed to the hexagonal structure and strong acidic nature of FSM-16.