In this paper, the effects of zinc (Zn) and magnesium (Mg) addition on the performance of an aluminum-based sacrificial anode in seawater were investigated using a potential measurement method. Anodic efficiency, protection efficiency, and polarized potential were the parameters used. The percentages of Zn and Mg in the anodes were varied from 2% to 8% Zn and 1% to 4% Mg. The alloys produced were tested as sacrificial anodes for the protection of mild steel in seawater at room temperature. Current efficiency as high as 88.36% was obtained in alloys containing 6% Zn and 1% Mg. The polarized potentials obtained for the coupled (steel/Al-based alloys) are as given in the Pourbaix diagrams, with steel lying within the immunity region/cathodic region and the sacrificial anodes within the anodic region. The protection offered by the sacrificial anodes to the steel after the 7th and 8th week was measured and protection efficiency values as high as 99.66% and 99.47% were achieved for the Al-6%Zn-1%Mg cast anode. The microstructures of the cast anodes comprise of intermetallic structures of hexagonal Mg3Zn2 and body-centered cubic Al2Mg3Zn3. These are probably responsible for the breakdown of the passive alumina film, thus enhancing the anode efficiency.