Carbon dioxide is known as a hazardous material with acidic property that can be found as impurity in natural gas reservoirs with a broad range of 2 up to 40 %. Therefore, many efforts have been directed to remove and separate carbon dioxide from methane to prevent corrosion problems as well as improving the natural gas energy content. In this study, two molecular sieves, silicoaluminophosphate-34 (SAPO-34) zeotype and T-type zeolite, were synthesized by the hydrothermal method for the comparative study of adsorptive separation of carbon dioxide from methane. The synthesized adsorbents were characterized by X-ray diffraction, scanning electron microscopy, energy dispersive X-ray spectroscopy, and Brunner–Emmett–Teller techniques. These characterization tests confirmed formation of both materials with acceptable crystallinity. Both adsorbents were tested in equilibrium adsorption experiments in order to evaluate maximum capacity and adsorption affinity. Adsorption capacity of carbon dioxide and methane on SAPO-34 and zeolite T were measured in a pressure range of 0.1–2.0 MPa and temperature of 288, 298, and 308 K and fitted with the Sips and Langmuir isotherm models. The ideal selectivity of CO2/CH4 was determined for SAPO-34 and zeolite T at the studied pressures and temperatures, indicating that the molecular sieves can be properly used for CO2–CH4 separation or CO2 capturing from natural gas.