In this study, experiments were performed to clarify the grain-refining mechanisms of pure Mg cast by adding some grain refiners containing Al3Ti, TiC, TiB2, and AlB2 particles as heterogeneous nucleation sites. It is found that Al–5 mass % Ti, Al–3 mass % Ti–0.15 mass % C, Al–5 mass % Ti–0.2 mass % B, and Al–5 mass % Ti–1 mass % B alloys are effective grain refiners for pure Mg, as well as for pure Al and Al alloys. The favourable heterogeneous nucleation sites in these refiners are considered to be TiC, TiB2, and AlB2 particles.