Decontamination of spent nuclear fuel from decommissioned nuclear reactors is crucial to reduce the volume of intermediate-level waste. Fuel cladding hulls are one of the important parts due to high radioactivity. Their decontamination could possibly enable reclassification as low-level waste. Fuel cladding hulls used in research reactors and being developed for conventional light water reactors are Al-Mg and Fe-Cr-Al alloys, respectively. Therefore, the recovery of these component metals after decontamination is necessary to reduce the volume of highly radioactive waste. Electrochemical approach is often chosen due to its simplicity and effectiveness. Non-aqueous solvents, such as molten salts (MSs) and ionic liquids (ILs), are preferred to aqueous solvents due to the absence of hydrogen evolution. However, MSs and ILs are limited by high temperature and high synthesis cost, along with toxicity issues. Deep eutectic solvents (DESs) are synthesized from a hydrogen bond acceptor (HBA) and donor (HBD) and exhibit outstanding metal salt solubility, wide electrochemical window, good biocompatibility, and economic production process. These characteristics make DES an attractive candidate solvent for economic, green, and efficient electrodeposition compared with aqueous solvents such acids or nonaqueous solvents such as MSs or ILs. In this research, the feasibility of electrodeposition of Al-Mg and Fe-Cr-Al alloys in ChCl:EG, the most common DES synthesized from choline chloride (ChCl) and ethylene glycol (EG), will be tested. A standard three-electrode electrochemical cell with an Au plated working electrode and Al wires for counter and reference electrodes is utilized. Two electrolyte solutions (Al-Mg and Fe-Cr-Al) are prepared by dissolving 100 mM of each anhydrous metal chloride salts (AlCl3, MgCl2, CrCl3, and FeCl2) in ChCl:EG. Cyclic voltammogram (CV) is measured at 5, 10, 15, and 20 mV·s−1 to observe the redox reactions occurring in the solutions. Electrodeposition of each alloy is performed via chronoamperometry at observed reduction potentials from CV measurements. The deposited surfaces and cross-sections are examined by scanning electron microscopy and energy dispersive spectroscopy (SEM-EDS) to analyze the surface morphology, cross-section composition, and thickness. Authors anticipate that the presence of different metals will greatly affect the possibility of electrodeposition. It is expected that although all metals are distributed throughout the surface, the morphology, in terms of particle size and shape, would differ depending on metals. Different metals will be deposited by layers of an approximate thickness of a few μm each. This research will illustrate a potential for recovery and electrodeposition of other precious radioactive metals from DES.