New experimental data for adsorption of ethylene and ethane on zeolite 13X and zeolite 5A are reported at a temperature range of 288-308 K and pressure up to 20 bar. The cation exchange for zeolites 13X and 5A was performed using copper, and the observed adsorption capacities of the copper-exchanged zeolites were measured. The equilibrium adsorption capacities of these adsorbents toward ethylene and ethane were compared. The copper-exchanged zeolites showed improved adsorption capacities toward both gases, where CuA was found to have the highest adsorption capacity. However, the copper-exchanged zeolites 13X and 5A underperformed in comparison to the expected high selectivity for ethylene/ethane separation. The data utilized for expressing the adsorption isotherm were successfully correlated with the Toth model, and the parameters for this model were calculated as reported in this paper.