A novel idea of precisely constructing gradient heterogeneous microstructure was proposed to greatly improve the formability of Al-Zn-Mg-Cu alloy by coupling multi-process firstly. After coupling control of the heterogeneous distribution of precipitates, strain energy storage and dislocation number density, a gradient distribution of coarse/fine grains can be constructed in the pre-aged alloy, resulting in a greatly enhanced average plastic strain ratio of 0.716. This work opens up a new frontier for achieving super-high room temperature formability without sacrificing the high strengths for Al-Zn-Mg-Cu alloys. GRAPHICAL ABSTRACT IMPACT STATEMENT This paper reports a gradient heterogeneous structure in Al-Zn-Mg-Cu alloys by coupling control of precipitates, strain energy storage and dislocation number density, resulting in a greatly enhanced average plastic strain ratio of 0.716.