In this study, the coating of an Al-Cr layer on the surface of a Zircaloy-4 alloy was carried out through plasma pretreatment coating and a laser surface melting process. Two different conditions for laser treatment, severe or minimal surface melting of the Zr alloy substrate, were applied to form the final coating. When there was significant surface melting of the Zr alloy, the solidification microstructure of the newly formed coating layer was mainly composed of needle-shaped Al3Zr, Al(Cr) and Al7Cr phases. On the other hand, the solidification microstructure of the coating layer was mainly composed of Al(Cr) and Al7Cr phases when there was minimal surface melting of Zr base in the laser process. However, when the coating was maintained at 1100 oC for 2 hours, significant inter-diffusion occurred between the phases in the coating. As a result, the upper part of the coating layer was observed to mainly consist of Al3Zr and Al8Cr5 phases, regardless of the laser treatment conditions.