Studies were carried out systematically on a series of Al-8.5 wt pct Zn-xMg-yCu alloys (x is about 1.5, 2.0, and 2.5 wt pct, and y is about 1.5, 2.0, 2.5, and 2.9 wt pct). The effects of alloying elements Mg and Cu on the microstructures of as-cast and homogenized alloys were investigated using the computational/experimental approach. It shows that Mg(Zn,Al,Cu) 2 (r) phase can exist in all the as-cast alloys without any observable Mg 32 (Al,Zn) 49 /Al 2 Mg 3 Zn 3 (T) or Al 2 CuMg (S) phase, whereas Al 2 Cu (h) phase is prone to exist in the alloys with low Mg and high Cu contents. Thermodynamic calculation shows that the real solidification paths of the designed alloys fall in between the Scheil and the equilibrium conditions, and close to the former. After the long-time homogenization [733 K (460°C)/168 hours] and the two-step homogenization [733 K (460°C)/24 hours + 748 K (475°C)/24 hours], the phase components of the designed alloys are generally consistent with the calculated phase diagrams. At 733 K (460°C), the phase components in the thermodynamic equilibrium state are greatly influenced by Mg content, and the alloys with low Mg content are more likely to be in single-Al phase field even if the alloys contain high Cu content. At 748 K (475°C), the dissolution of the second phases is more effective, and the phase components in the thermodynamic equilibrium state are dominated primarily by (Mg + Cu) content, except the alloys with (Mg + Cu) Z 4.35 wt pct, all designed alloys are in single-Al phase field.