As the need for global decommissioning and site remediation of aging and shut-down nuclear power plants continues to grow, it becomes increasingly crucial to efficiently treat contaminated soil while minimizing waste generation. This study explores an innovative soil decontamination approach that utilizes supercritical carbon dioxide (SCCO2) as the primary solvent, along with ethanol as a co-solvent and specific additives, including a chelate ligand (catechol ligand) and a co-ligand (NEt4PFOSA). The advantages of SCCO2, such as its penetration and solubility, coupled with its ability to separate from radioactive waste, are harnessed in this research. The study demonstrates that the combination of SCCO2, ethanol, and additives significantly enhances decontamination efficiency, particularly for cesium (Cs), strontium (Sr), and uranium (U) contamination. Results indicate that decontamination efficiency varies with soil particle size, with smaller particles presenting greater challenges. This study presents a promising eco-friendly soil decontamination technology using SCCO2 containing ethanol and specific additives to efficiently reduce radioactive contamination in soil.