In order to obtain high-strength and high-ductility Al-Si-Cu-Mg alloys, the present research is focused on optimizing the composition of soluble phases, the structure and morphology of insoluble phases, and artificial ageing processes. The results show that the best matches, 0.4 wt% Mg and 1.2 wt% Cu in the Al-9Si alloy, avoided the toxic effect of the blocky AlCu on the mechanical properties of the alloy. The addition of 0.6 wt% Zn modified the morphology of eutectic Si from coarse particles to fine fibrous particles and the texture of Fe-rich phases from acicular β-Fe to blocky π-Fe in the Al-9Si-1.2Cu-0.4Mg-based alloy. With the optimization of the heat treatment parameters, the spherical eutectic Si and the fully fused β-Fe dramatically improved the ultimate tensile strength and elongation to fracture. Compared with the Al-9Si-1.2Cu-0.4Mg-based alloy, the 0.6 wt% Zn modified alloy not only increased the ultimate tensile strength and elongation to fracture of peak ageing but also reduced the time of peak ageing. The following improved combination of higher tensile strength and higher elongation was achieved for 0.6 wt% Zn modified alloy by double-stage ageing: 100 °C × 3 h + 180 °C × 7 h, with mechanical properties of ultimate tensile strength (UTS) of ~371 MPa, yield strength (YS) of ~291 MPa, and elongation to fracture (E%) of ~5.6%.