Laser surface remelting (LSR) is a laser-based surface treatment method. In the LSR process, microstructural defects such as cracks and porosity are suppressed in addition to grain refinement, and the mechanical properties are improved. The present research investigated the effects of LSR parameters on the microstructure, wear, and corrosion behavior of Mg AZ80 alloy. The results showed that in LSR, the coarse-grained (29.8 μm) structure of AZ80 was transformed into a fine-grained structure (3.1 μm) with no microstructural defects. The evaporation of Mg during LSR and the formation of Al-rich and Mg-poor phases are the most important challenges in the surface treatment of AZ80. This limitation was solved by optimizing the LSR parameters, which included a gas flow rate of 2 L min−1, pulse duration of 3 ms, scanning speed of 3 mm s−1, pulse frequency of 8 Hz, and heat input of 64 J mm−1. The prevention of Mg evaporation was associated with the elimination of porosity and cracks, reducing of the solidification range, and uniform distribution of β-Mg17Al12 precipitation phases in α-Mg refined grains. The tribological behavior of the laser-treated region showed that the COF, depth of the wear scar, wear rate, and wear volume loss were reduced by 18%, 48%, 37%, and 66%, respectively, compared to AZ80. This result is attributed to the refinement of α-Mg grains and the uniform distribution of β-Mg17Al12 in the laser-treated region. The results of the polarization curves of the corrosion test in 3.5 wt% NaCl solution showed that the optimal laser-treated region with the lowest corrosion current density (34.68 × 10−6 μA.cm−2) and highest self-corrosion potential (1.425 V) exhibited the highest corrosion resistance. A slight change in the breakdown potential current slope in the laser-treated region indicates the formation of a protective film on the surface after the completion of LSR, which increases corrosion resistance.
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