In this study, a carbon molecular sieve (CMS) was synthesized from walnut shells, followed by physical activation of the carbon content of the CMS. Adsorption of CO 2 and CH 4 onto raw and acid treated adsorbents were investigated using two sizes, 300-600 and 600-1180 μm. The adsorbents were impregnated with two solvent mixtures of waste engine oil with kerosene and with thinner at a proportion of 1:1 at 25 °C. The highest adsorption for CO 2 and CH 4 was obtained at the suitable size of a group of CMS (A) adsorbents, with acid treated adsorbents being more efficient than the raw adsorbents. The acid treated CMS (A-3) sample adsorbed 0.925 mol CO 2 g-1 and 0.353 mol CH 4 g-1. The results indicated that by decreasing the granulation size of group CMS (R) adsorbents, the adsorption capacities for CO 2 and CH 4 were reduced while increasing the granulation size of group CMS (A) adsorbents resulted in an enhancement in the adsorption capacity for CO 2 and CH 4. Moreover, acid treated adsorbents achieved enhanced adsorption capacity for CO 2 and CH 4. Further modifications reduced the adsorption capacity for CO 2 and CH 4 in impregnated adsorbents, due to a decrease in surface area, pore volume and pore size of the adsorbent.