Vanadium oxide supported on MSU-1, with VO x loading ranging from 2.5 to 17.5 wt. %, was developed as a highly active catalyst in dehydrogenation of isobutane with CO 2 . The obtained catalysts of VO x /MSU-1 were characterized by X-ray diffraction (XRD), N 2 adsorption-desorption, and H 2 -temperature programmed reduction (H 2 -TPR) methods and the results showed that the large surface area of MSU-1 was favorable for the dispersion of VO x species and the optimal loading of VO x was 12.0 wt. %. Meanwhile, the catalytic activity of VO x /MSU-1 was investigated, and VO x /MSU-1 with 12.0 wt. % VO x content was found to be the best one, with the conversion of isobutane (58.8%) and the selectivity of isobutene (78.5%) under the optimal reaction conditions. In contrast with the reaction in the absence of CO 2 , the presence of CO 2 in the reaction stream could obviously enhance the isobutane dehydrogenation, which raised the conversion of reaction and the stability of VO x /MSU-1.