Friction stir processing (FSP) of as-cast Mg-7Al, Mg-4Al-3Ca (AX43), and Mg-2Al-5Ca (AX25) magnesium alloys led to the remarkable grain refinement and enhancement of mechanical properties. This is due to the replacement of the interconnected, brittle constituents with uniformly dispersed fine particles after FSP. Due to the presence of thermally-stable Al-Ca intermetallics, the calcium-containing alloys showed more intense grain refinement compared to the Mg-7Al alloy with unstable Mg17Al12 phase. The friction stir processed AX43 alloy with a grain size of 1.7 μm exhibited the best tensile properties.