Considering the necessity of the development of methods to reduce the burden of storage and disposal of high-level radioactive waste, in this study, we propose a nuclide separation technique using molten salt immersion. The dissolution behavior of simulated spent nuclear fuels (SSFs) immersed in a LiCl-KCl-UCl3 (LKU) molten salt at 500°C was investigated using a combination of thermodynamic and experimental studies. Surrogates of transuranic elements (TRUs), that is, rare earth elements (REs), in the SSFs were dissolved into the molten salt without any damage to the UO2 structure of the SSFs. The results suggest that the LKU salt technique can be used to separate REs and, potentially, TRUs from actual spent nuclear fuels (SNFs). It is thought that this technique is advantageous over the conventional TRU recovery techniques because the majority of the SNFs (i.e., UO2) remained stable, thus reducing the process burden. Several SNF treatment process options using this technique were suggested. This study will serve as a guide for future studies on the management of high-level waste discharged from nuclear reactors.