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The smart detection of concrete-corrosivity and the intelligent protection of reinforcing steel provided by Mg alloys with various Al contents were systematically investigated in a reconstituted concrete pore solution (RCPS). The results indicated that increasing the Al concentration of the alloy up to 17 wt% could enhance the performance of corrosivity-detection and the corrosion-protection. However, excessive Al alloying could lead to an over-protection of the steel. The optimized Mg-Al alloy sensing and protecting anode was also verified in mortar prisms. Based on these findings, the anodic behaviors of Mg-Al alloys in the RCPS were analyzed.