Carbon capture by physical adsorption can strongly participate in the reduction of the carbon dioxide emissions from the flue gases with minimum energy penalties. In this paper, we report the experimental data for enhancing the adsorption separation capability of zeolite 13X incorporated with carbon nanotubes (CNT). Six samples (13X, XC1, XC2, XC3, XC4, and XC5) have been characterized by XRD. Equilibrium adsorption isotherms and actual dynamic behavior of adsorption breakthrough tests were conducted. XRD analyses show that all the samples have almost identical XRD patterns to pure 13X, while the equilibrium isotherms indicate that XC3 (0.5 wt% CNT/13X) has CO2 adsorbed amounts much closer to those of pristine 13X. Interesting results of actual capturing behavior were exposed during the breakthrough tests which confirm that the optimal adsorption separation is associated with XC3 with an increased adsorption capacity and separation breakpoint by about 21.4 and 25.3%, respectively, in comparison to pure 13X.