The effects of trace Sc, Zr, and Ti on the microstructure and hardness of Al alloys with high Mg content (Al-6Mg, Al-8Mg, and Al-10Mg) were studied by optical microscope, scanning electron microscopy (SEM), transmission electron microscopy (TEM), and Brinell hardness. The grain size of the as-cast alloys was refined by the addition of Sc and Zr, and it was further refined by the addition of Ti. With the same contents of Sc, Zr, and Ti, an increase in Mg content was beneficial to the refinement due to the solution of Mg into α-Al. The refined microstructures of the as-cast alloys were favorable for Brinell hardness. Addition of Sc, Zr, and Ti to the Al-10Mg alloy results in the improvement of peak hardness and it is about 45% higher than that of the Al-10Mg alloy, which is due to fine precipitations of