Disclosed herein is a clay-alkali-amine CO2 sorbent composition prepared by integrating a clay substrate, basic alkali salt, and amine liquid. The basic alkali salt is present relative to the clay substrate in a weight ratio of from about 1 part to about 50 parts per 100 parts of the clay substrate. The amine liquid is present relative to a clay-alkali combination in a weight ratio of from about 1 part to about 10 parts per 10 parts of the clay-alkali combination. The clay-alkali-amine C02 sorbent is particularly advantageous for low temperature CO2 removal cycles in a gas stream having a C02 concentration less than around 2000 ppm and an oxygen concentration around 21%, such as air.