A series of Mg-Al-CO3 layered double hydroxide (LDH) samples have been synthesized by conventional precipitation and coprecipitation methods. The effect of various synthetic parameters, such as cation molar ratio, mode of addition of magnesium and aluminum precursors, addition temperature, agitation, and drying conditions, on the structural, textural, and thermal behavior of the samples has been studied. These properties were correlated with the CO2 adsorption capacity of the samples. The Mg-Al-CO3 LDH sample prepared with optimized synthetic parameters has shown the higher CO2 adsorption capacity (22 cm(3)/g).