This paper proposes a new high-strength Al-Zn-Mg-Ni alloy with excellent twin-roll castability compared with conventional Al-Zn-Mg-Cu alloys. Thermodynamic calculations were carried out to identify the solidification range and amount of residual liquid phase in the Al-Zn-Mg-(Cu, Ni) alloys, which are factors exerting significant influence on the formation of defects in the final strips. The designed Al-Zn-Mg-Ni alloys exhibited a narrower solidification range and smaller amount of residual liquid at the final solidification temperature, resulting in excellent surface quality after twin-roll casting compared with Al-Zn-Mg-Cu alloys. A series of rolling and heat treatment processes was performed on the Al-Zn-Mg-Ni alloy strips, and the mechanical properties of the final sheets were evaluated. The results showed that the yield and tensile strength were increased without affecting the elongation up to approximately 1.0wt.% Ni addition. Additionally, compared with conventional Al-Zn-Mg-Cu alloys, equivalent or higher tensile properties were achieved after T6 tempering. In conclusion, the Al-Zn-Mg-Ni alloy exhibits high-strength with excellent twin-roll castability.