Cr-MCM-41 synthesized by both direct hydrothermal (DHT) and template-ion exchange (TIE) methods is studied for dehydrogenation of lower alkanes including C2H6, C3H8 and i-C4H10 with CO2. Both methods lead to Cr species highly dispersed on the wall surface of MCM-41 and exhibited similar catalytic behaviors. Selectivity higher than 90% to each alkene has been achieved, and the presence of CO2 enhances the conversion of alkane.