A mixed salt composition adapted for use as a sorbent for carbon dioxide removal from a gaseous stream is provided, the composition being in solid form and including magnesium oxide, an alkali metal carbonate, and an alkali metal nitrate, wherein the composition has a molar excess of magnesium characterized by a Mg:X atomic ratio of at least about 3:1, wherein X is the alkali metal. A process for preparing the mixed salt is also provided, the process including mixing a magnesium salt with a solution comprising alkali metal ions, carbonate ions, and nitrate ions to form a slurry or colloid including a solid mixed salt including magnesium carbonate; separating the solid mixed salt from the slurry or colloid to form a wet cake; drying the wet cake to form a dry cake including the solid mixed salt; and calcining the dry cake to form a mixed salt sorbent.