In this study, the effects of compound modification with Bi and Sb and solution treatment on the microstructures evolution and the mechanical properties of Al-20 wt.% Mg2Si composites were investigated. The specimens were observed by optical microscope, scanning electron microscope equipped with an energy-dispersive spectrometer and x-ray diffraction. The characterization results showed that 2.0 wt.% Sb and 0.2 wt.% Bi addition refined the primary Mg2Si from 95 to 10 μm, accompanied by a change in morphology from coarse dendrites to dispersive fine polygons. After solution treatment at 540 °C for 15 h, the sharp polygonal primary Mg2Si particles were blunted and the flake-like eutectic Mg2Si phases were changed to small spherical particles, resulting in the increase in the Brinell hardness of the composites from HB 94.53 to 134.67. Mechanical tests revealed that both tensile strength and hardness of the composite were improved by compound modification with Bi and Sb, and the ultimate tensile strength (UTS) was increased from 216 MPa unmodified to 257 MPa with optimum modification of 2 wt.% Sb and 0.2 wt.% Bi. A propounded change in hardness from HB 94.53 to 130.67 was also investigated.