The grain size of magnesium solid-solution alloys with lithium, indium, and/or zinc has been determined. Lithium, indium, and zinc additions decreased the grain size, D, of magnesium solid-solution alloys cast in a copper mold. The most effective grain refinement was obtained by zinc. In binary Mg–Zn alloys, grain size is related to the growth restriction factor, Q as D = 94 + 312/Q. In Mg–Li and Mg–In binary alloys, grain size versus growth relationships described as D = a + b/Q indicated that these alloys have lower numbers of nucleants but with higher potency than the Mg–Zn binary system. For Mg–Li and especially Mg–In, grain size could be related to growth restriction as D = 383Q−n with higher R2. Ternary and quaternary alloys based on Mg–Zn with Li and/or In additions also follow the D = a + b/Q relationship with the parameters indicating a larger number of lower potency nucleants than the Mg–Zn binary alloys. Electron probe microanalysis showed that Mg–Zn alloys exhibit pronounced and persistent grain-boundary enrichment of Zn, pointing toward Scheil solidification.