In this study, ZnO was synthesized by the simple hydrothermal method. The physicochemical properties of the materials were characterized by SEM, XRD, N adsorption/desorption isotherm methods. The CO2 removal experiments were conducted using the thermogravimetric method (TGA). The material has a stratified structure, with a surface area of 24.4 m2/g and a pore volume of 0.280 cm3/g. The influences of temperature, ZnO morphology, and feed gas composition were studied. Besides, the durability and applicability of the material were evaluated through repeated regeneration.