The adsorption capacities of carbon dioxide on six commercial hydrotalcite-like compounds and the main factors (aluminum content, anion type, water content, and heat treatment temperature) influencing their adsorption capacity at high temperatures have been investigated using a gravimetric technique. There is an optimum aluminum content and heat treatment temperature for the adsorption capacity. The carbonate anion favors adsorption of carbon dioxide compared to OH-, and a low content of water also improves the adsorption capacity. The carbon dioxide adsorption capacity is mainly dependent on the microporous volume, interlayer spacing, and layer charge density of the hydrotalcite-like compounds.