In the oxidative dehydrogenation of isobutane to isobutene, selectivity and stability were improved by introducing chromium and molybdenum into SBA-15. The direct synthesis method (DM) was used to introduce these binary elements into SBA-15. Use of the DM resulted in a higher specific surface area of the catalyst and a greater dispersion of chromium and molybdenum species compared with a corresponding binary catalyst prepared using the incipient wetness impregnation method (IM). Selectivity to isobutene was improved, along with a decrease in the selectivities to CO and CO2 with the introduction of greater amounts of molybdenum, which suggests that molybdenum must suppress the tendency of isobutene to over-oxidate to either CO or CO2. The molybdenum species must be in close proximity to the chromium species, which results in the formation of an active Cr-O-Mo site.