The role of bismuth (50 to 9000 ppm) and calcium (50 to 200 ppm) additions on the microstructural characteristics in Sr-modified 319 alloys (with/without 0.4 wt% Mg addition) were investigated using optical and electron microscopy, and image analysis. It was found that the modification effect of Sr continuously diminished with Bi addition up to similar to 3000 ppm Bi; further Bi addition led to the modification of the Si particles due to the presence of Bi. In the Ca-containing alloys, a coarse eutectic Si structure resulted with Ca additions of 50 ppm, due to the formation of Al-x(Ca,Sr)Si-y compounds. Increased Ca additions (up to 200 ppm) did not alter the Si particle size. The Al-x(Ca,Sr)Si-y phase particles appeared in rod-like form in the Sr-modified alloys and in plate-like form in the 319+0.4 wt% Mg alloys. MgO, Al2O3, and AlP particles appear to act as nucleants for the precipitation of the plate-like Al-x(Ca,Sr)Si-y phase.