Perovskite-supported alkaline-earth metal oxide catalysts were prepared for application in the oxidative coupling of methane (OCM). The selective production of C2+ compounds, including ethane, ethylene, acetylene, propane, and propylene, was observed at reaction temperatures <700 degrees C. This lower reaction temperature was not achieved with pure perovskites but only with the combination of alkaline-earth metal oxides and perovskite supports. The formation of complex mixed oxides, such as Ba-Ca-Ti-O-x, Ba-Sr-Ti-Ox, and Ba2TiO4, was also observed for these catalysts. This contributed to the improved C2+ yield at the lower reaction temperature. The strong basicity, which contributes to the improved OCM activity, was also observed for these catalysts.