In the present experimental investigation, Al-3 wt%Cu and Al-3 wt%Cu-0.5 wt%Mg alloys castings are produced by a horizontal solidification technique with a view to examining the interrelationship among growth rate (G R ), cooling rate (C R ), secondary dendrite arm spacing (k 2 ), Vickers microhardness (HV), and corrosion behavior in a 0.5 M NaCl solution. The intermetallic phases of the as-solidified microstructures, that is, h-Al 2 Cu, S-Al 2 CuMg, and x-Al 7 Cu 2 Fe, are subjected to a comprehensive characterization by using calculations provided by computational thermodynamics software, optical microscopy, and scanning electron microscopy/energy-dispersive spectroscopy. Moreover, electrochemical impedance spectroscopy and potentiodynamic polarization tests have been applied to analyze the corrosion performance of samples of both alloys castings. Hall-Petch-type equations are proposed to represent the HV dependence on k 2 . It is shown that the addition of Mg to the Al-Cu alloy has led to a considerable increase in HV; however, the Al-Cu binary alloy is shown to have lower corrosion current density (i corr ) as well as higher polarization resistance as compared to the corresponding results of the Al-Cu-Mg ternary alloy.