The CO 2 capture properties of M 2 CO 3 (M = Na, K)-promoted and CaCO 3 -promoted MgO sorbents are investigated by first-principles density functional theory complemented with lattice phonon calculations. The calculated thermodynamic properties indicate that by forming double salts (M 2 Mg(CO 3 ) 2 and CaMg(CO 3 ) 2 ), compared to pure MgO, the maximum allowable CO 2 capture temperatures of the M 2 CO 3 -and CaCO 3 -modified MgO sorbents are shifted to higher temperature ranges. Under pre-combustion conditions with P CO 2 = 10 bar, the Na 2 CO 3 -promoted and CaCO 3 -promoted MgO sorbents can capture CO 2 at temperatures as high as 915 K and 740 K respectively. While under post-combustion conditions with P CO 2 = 0.1 bar, their maximum allowable CO 2 capture temperatures are 710 K and 600 K respectively. However, when adding K 2 CO 3 into MgO, under both pre-and post-combustion conditions, its maximum CO 2 capture temperatures only increased about 10 K relative to pure MgO. These results indicate that by mixing another solid into MgO, it is possible to shift its CO 2 capture temperature to fit practical industrial needs.