The ultralight hypoeutectic a-phase Mg-4.5Li-1.5Al alloy and hypereutectic b-phase Mg-12Li-1.5Al alloy in as-cast state were fabricated and subjected to modification by 0.2 mass% TiB and 0.2 mass% Sr grain modifiers. The crystallisation sequence of Mg-Li-Al alloys has been investigated in detail by using thermal-derivative analysis and microstructural observations. The presented work includes the effects of grain refiners on grain size and microstructure and thermal events registered during crystallisation of ultralight Mg-Li-Al alloys by recording and analysis of the temperature vs time, i.e. as T N , T a , T b , T g(LiAl) and T SOL. Microstructure and phase observation has been done by light microscope, X-ray diffraction and energy dispersive X-ray spectroscopy. The changes of characteristic temperature points for phase transformation are studied in detail. Due to the addition of 0.2 mass% TiB and 0.2 mass% Sr, the grain structure of the alloy was refined, and mechanical properties were improved. When a TiB and Sr added simultaneously, the average grain size of the analysed alloys strongly decreases. When the TiB or Sr content was severally added, a low effect of improvements of mechanical properties was observed. With the TiB and Sr content, the liquidus and solidus decrease gradually.