An accumulation of spent nuclear fuel (SNF) has brought a considerable interest due to its energy and environmental issue. To effectively manage SNF, a pyroprocessing is introduced to separate useful resources from the spent fuels and to manufacture suitable fuels. In head-end process of pyroprocessing, spent fuels are thermally treated to prepare UO2 pellets, where various radioactive gases from SNFs are released during thermal treatment. Within these gases, C-14 as CO2 form is a radioactive fission product which had a long half-life of 5,730 years and emits beta radiation of 0.156 MeV. Generally, current CO2 capturing technologies include adsorption by solid materials, absorption by aqueous solutions, and membrane separation. Among these methods, absorption is an effective approach which traps CO2 effectively and and it is easy to operate at room temperature. In addition, it is highly recommended as immobilizing 14CO2 as CaCO3 formation due to the high thermal and chemical stability, and the relatively low solubility in water. Generally, a double alkali method has been proposed to capture low concentrated 14CO2 from the stream. This method for CO2 capture includes absorption process with NaOH solution and causticization using Ca(OH)2. In this study, CO2 emitted from SNF is captured using double alkali method, and the effects of operating conditions on capturing efficiency were investigated. Furthermore, considering the two-film theory, the effects of trapping conditions on the CO2 absorption performance were examined. The recovered CaCO3 from causticization was collected from the absorbing solution and analyzed.