Nickel–chromium (NiCr) alloys are characterized by their strong resistance to corrosion, wear resistance, and hardness. Owing to these properties, the Ni-Cr electrodeposition is a topic of current interest. In this work, electrodeposition processes of Ni-Cr alloys onto a glassy carbon electrode from a eutectic mixture, formed by mixing choline chloride and urea with 1:2 mol ratio (reline), were studied by electrochemical means. Voltametric results have shown the capability of the nickel-chromium electrodeposition from the reline DES with one (two-electrons) reduction step. Analyses of the current density transients demonstrated that nickel-chromium electrocrystallization could follow 3D nucleation and control by diffusion mechanisms on the bimetallic growing surface. Also, it was found that the Ni(II) component plays a vital role during the nickel-chromium electrodeposition, which contributes to the fast kinetics of nickel-chromium phase formation from the reline DES. Surface characterization methods verified the evidence of the nickel-chromium phase formation and its crystal structure, respectively. The excellent quality of nickel-chromium alloys obtained from DES offers important applications of this alloy in different engineering fields, such as surface coating and metal protection.