In the dehydrogenation of ethylbenzene to styrene, CO2 could play a role as an oxidant to increase conversion of ethylbenzene and stability as well over TiO2-ZrO2 mixed oxide catalysts. TiO2-ZrO2 catalysts were prepared by co-precipitation method and were characterized by BET surface area, bulk density, X-ray diffraction, temperature programmed desorption of NH3 and CO2. These catalysts were found to be X-ray amorphous with enhanced surface areas and acid-base properties both in number and strength when compared to the respective oxides (TiO2 and CO2). These catalysts were found to be highly active (> 50% conversion), selective (> 98%) and catalytically stable (10 h of time-on-stream) at 600 oC for the dehydrogenation of ethylbenzene to styrene. However, in the nitrogen stream, both activity and stability were rather lower than those in the stream with CO2. The TiO2-ZrO2 catalysts were catalytically superior to the simple oxide catalysts such as TiO2 and ZrO2. The synergistic effect of CO2 has clearly been observed in directing the product selectivity and prolonging catalytic activity.