Today, the domestic and international nuclear power industry is experiencing an acceleration in the scale of the nuclear facility decommissioning market. This phenomenon is also due to policy changes in some countries, but the main reason is the rapid increase in the proportion of old nuclear power plants in the world, mainly in countries that introduced nuclear power plants in the early stages. Decontamination is essential in the process of decommissioning nuclear facilities. Among various decontamination targets, radionuclides are adsorbed between pores in the soil, making physical decontamination quite difficult. Therefore, various chemical decontamination technologies are used for contaminated soil decontamination, and the current decontamination technologies have a problem of generating a large amount of secondary wastes. In this study, soil decontamination technology using supercritical carbon dioxide is proposed and aimed to make it into a process. This technology applies cleaning technology using supercritical fluids to decontamination of radioactive waste, it has important technical characteristics that do not fundamentally generate secondary wastes during radioactive waste treatment. Supercritical carbon dioxide is harmless and is a very useful fluid with advantages such as high dissolution, high diffusion coefficient, and low surface tension. However, since carbon dioxide, a non-polar material, shows limitations in removing polar and ionic metal wastes, a chelating ligand was introduced as an additive. In this study, a ligand material that can be dissolved in supercritical carbon dioxide and has high binding ability with polar metal ions was selected. In addition, in order to increase the decontamination efficiency, an experiment was conducted by adding an auxiliary ligand material and ultrasonic waves as additives. In this study, the possibility of liquefaction of chelating ligands and auxiliary ligands was tested for process continuity and efficiency, and the decontamination efficiency was compared by applying it to the actual soil classified according to the particle size. The decontamination efficiency was derived by measuring the concentration of target nuclides in the soil before and after decontamination through ICP-MS. As a result of the experiment, it was confirmed that the liquefaction of the additive had a positive effect on the decontamination efficiency, and a difference in the decontamination efficiency was confirmed according to the actual particle size of the soil. Through this study, it is expected that economic value can be created in addition to the social value of the technology by ensuring the continuity of the decontamination process using supercritical carbon dioxide.