Copper nanosheets and sulfur particles were synthesized synchronously by electrolysis, after dissolving Cu₂S in ChCl–thiourea (TU) deep eutectic solvent (DES) system. The optimized electrolysis conditions of 0.9 V, 80 °C, and 2 h resulted in the deposition of pure nano-sized copper sheets with a length of approximately 500 nm and a thickness of approximately 30 nm, and the production of sulfur particles with an average size of approximately 10 μm. The morphology of the cathodic products was significantly influenced by the electrolysis voltage. When Cu₂S was introduced into ChCl-TU, it dissolved [CuCl₂]^- without disrupting the structure of the choline ion (Ch⁺). As the electrolysis time increased, the copper deposition changed from wire to sheet growth, with the growth direction from radial to epitaxial along the substrate and back to radial.