Carbon dioxide (CO2) removal from natural gas attracts more attention than other impurities due to its corrosiveness property and it also possess no heating value in the sales natural gas. Amine based chemical absorption has been used commercially for CO2 separation in gas processing plant. However, the liquid amine based processes pose operating difficulties due to high regeneration energy, large equipments size and solvent leakage. This research studies modification of porous materials, zeolite NaY by grafting amine functional group using monoethanolamine directly to the surface of the solid sorbents. The structures and physical properties of amine modified adsorbent were characterized using powder X-Ray Diffraction (XRD), nitrogen adsorption at 77K and thermogravimetric analysis. Since application of Pressure Swing Adsorption (PSA) has been widely used in various plants in the world, this research was extended to study carbon dioxide separation using amine modified adsorbents in PSA experimental system. Effects of adsorption and regeneration behaviour on CO2 separation were investigated. Amine modified NaY showed better result compared to unmodified NaY in term of improvement in physical and chemical properties, high CO2 adsorption capacity and modified adsorbents were ease of regeneration.