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Dense Fe-Al-Cr coatings with approximately 50 μm in thickness are successfully prepared on the 1045 carbon steel substrates via a laser cladding process. Proper Cr content (5 at％ Cr) will lead to decrease in the melting point, and improves the viscosity of the liquid and the nucleation rate of the molten pool, leading to refining grains of the solidification structure. As a result, the Fe-29Al-5Cr laser cladding layer exhibits the best hardness, plasticity properties, and wear resistance at 400 °C. Excessive Cr for the Fe-29Al-7.5Cr coating leads to the formation of Cr2Al in the grain boundaries and thermal vacancies during the solidification process, resulting in inferior mechanical properties and poor tribological behavior.