<p>During zinc production via hydrometallurgical processes, a large volume of toxic residue is stockpiled annually. These wastes contain a considerable level of valuable metals, and it is logical to treat these wastes aiming to amplify the economic viability of the process besides the contamination reduction. During the cold purification stage, zinc dust is added to the leached solution to remove impurities such as Ni and Cd, forming a Cold Filter Cake (CFC), which poses an environmental risk if improperly stockpiled. In recent years, a new class of green solvents has emerged with unique traits, such as biodegradability and biocompatibility, which are known as Deep Eutectic Solvents (DESs). This study synthesized and applied a wide range of choline chloride (Ch)-based DESs as a leaching agent to dissolve the CFC. Ch-Ethylene Glycol, Ch-Urea, and Ch-Glucose solvents were ineffective in adequately leaching Ni, Cd, and Zn from the CFC. Ch-Oxalic solvent could selectively dissolve all of Cd from the CFC. Ch-Citric, Ch-Malonic, Ch-Maleic, and Ch-PTSA (p-toluenesulfonic acid) solvents are capable of successfully dissolving more than 80% of Ni, Cd, and Zn from the CFC. Among the evaluated solvents, Ch-Malonic exhibited superior metal solubilization performance. Fourier transform infrared spectroscopy analysis shows the formation and stability of Ch-Malonic DES during leaching. Also, characterization of CFC using a field emission scanning electron microscope coupled with an energy-dispersive X-ray spectroscopy was done before and after leaching in Ch-Malonic DES. Results showed that Ch-Malonic completely dissolved target metals. Hence, this solvent can be a favorable potential solvent for Ni, Cd, and Zn dissolution with a salient leaching efficiency. Interactions between metal ions (Ni²⁺_, Cd²⁺, Zn²⁺) and Ch-Malonic DES were investigated using COnductor-like Screening MOdel (COSMO) calculations and Radial Distribution Functions (RDF). The results suggest that chloride ions in choline chloride form stronger bonds with Zn²⁺ and Ni²⁺ compared to Cd²⁺, while Cd²⁺ exhibits a higher affinity for oxygen atoms within the OH bond of malonic acid, indicating a preference for oxygen-based complexes.</p> Graphical Abstract <p></p>