The increased levels of carbon dioxide in the environment have incited the search for breakthrough technologies to lessen its impact on climate. The CO2 capture from a mixture of CO2/N2 was studied using a molecular sieve (MS) and silica gel type-III. The breakthrough behavior was predicted as a function of temperature, superficial velocity, and CO2 partial pressure. The breakpoint time reduced significantly with increased temperature and increased superficial velocity. The CO2 adsorption capacity increased appreciably with decreased temperature and increased CO2 pressure. The saturation CO2 adsorption capacity from the CO2/N2 mixture reduced appreciably with increased temperature. The molecular sieve contributed to higher adsorption capacity, and the highest CO2 uptake of 0.665 mmol/g was realized for MS. The smaller width of the mass transfer zone and higher column efficiency of 87.5% for MS signify the efficient use of the adsorbent; this lowers the regeneration cost. The findings suggest that a molecular sieve is suitable for CO2 capture due to high adsorption performance owing to better adsorption characteristic parameters.