This study systematically investigates the influence of FeCl2 concentration on the electrochemical behavior of the AlCl3-BMIC (1-butyl-3-methylimidazolium chloride) ionic liquid system, aiming to optimize the electrolyte composition for the controllable electrodeposition of high-iron-content Fe-Al alloys. The variations in ionic conductivity and electrochemical reduction kinetics are analyzed via conductivity measurements and cyclic voltammetry (CV). The results demonstrate that the ionic conductivity of the AlCl3-BMIC-FeCl2 ionic liquid decreases linearly with increasing FeCl2 concentration. This phenomenon is attributed to the reaction between FeCl2 and [Al2Cl7]? to form bulky [Fe(AlCl4)4]2- complexes, which reduces the mobility of charge carriers. In contrast, conductivity exhibits a positive correlation with temperature, following the temperature-dependent Kohlrausch empirical formula. As the concentration increases from 10 mmol/L to 90 mmol/L, the activation energy for ionic migration slightly increases from 9.18 kJ/mol to 9.95 kJ/mol, which originates from the hindrance effect of the generated bulky [Fe(AlCl4)4]2- complex ions on ion transport. Cyclic voltammetry indicate that Fe(II) significantly inhibits the reduction of Al(III). With increasing FeCl2 concentration, the aluminum deposition potential shifts negatively, and the reduction peak current density decreases, this is directly related to the reduced concentration of the electroactive species [Al2Cl7]-. The Fe(II) reduction peak current density increases with FeCl2 concentration while its reduction potential shifts negatively, likely due to decreased activity of [Fe(AlCl4)4]2- ions and enhanced ion-pair interactions. A linear relationship between the Al(III) reduction peak current density and Fe(II) concentration reveals the inhibitory effect of Fe(II) on aluminum electrodeposition. Additionally, the potential difference between Fe(II) and Al(III) reduction gradually decreases with increasing FeCl2 concentration, facilitating the co-deposition of Fe-Al alloys. Based on this trends, Fe-Al alloys with Fe contents ranging from 13.5wt%~68.1wt% are successfully prepared by adjusting the FeCl2 concentration. Their microstructure exhibits a progressive evolution: from nodular aggregates to uniform microspheres and floral structures. These results highlight FeCl2 concentration as a key parameter for tailoring Fe-Al alloy composition and microstructure, enabling controllable synthesis of Fe-rich coatings for advanced applications.