Aluminum’s exceptional properties, such as its high strength-to-weight ratio, excellent thermal conductivity, corrosion resistance, and low neutron absorption cross-section, make it an ideal material for diverse nuclear industry applications, including aluminum plating for the building envelope of nuclear power plants. However, plating aluminum presents challenges due to its high reactivity with oxygen and moisture, thus, complicating the process in the absence of controlled environments. Plating under an inert atmosphere is often used as an alternative. However, maintaining an inert atmosphere can be expensive and presents an economic challenge. To address these challenges, an innovative approach is introduced by using deep eutectic solvents (DES) as a substitute for traditional aqueous electrolytes due to the high solubility of metal salts, and wide electrochemical window. In addition, DESs offer the benefits of low toxicity, low flammability, and environmentally friendly, which makes DESs candidates for industrial-scale applications. In this study, we employed an AlCl3-Urea DES as the electrolyte and investigated its potential for producing aluminum coatings on copper substrates under controlled conditions, for example, current density, deposition duration, and temperature. A decane protective layer, non-polar molecular, has been used to shield the AlCl3-Urea electrolyte from the air during the electrodeposition process. The electrodeposition was successful after being left in the air for two weeks. This study presents a promising and innovative approach to optimizing aluminum electrodeposition using deep eutectic solvents, with potential applications in various areas of the nuclear industry, including fuel cladding, waste encapsulation, and radiation shielding.