Supported MgO/γ-Al2O3 were prepared by a facile one-pot double hydrolysis method. The MgO/γ-Al2O3 show enhanced CO2 adsorption capacities under simulated flue gas. Mg/Al-0.2 shows a stable adsorption capacity after 11 cycles at 60 °C. Bicarbonate, bidentate and monodentate carbonate are formed during CO2 adsorption. Dynamic CO2 adsorption capacity increases with increasing the amount of basic sites.