The strength improvement in the heat-treatable Al-Zn-Mg-Cu alloys is generally achieved by increasing the volume fraction of nanoprecipitates and reducing the grain size. However, utilizing one of them usually leads to a drastic decrease in ductility. Herein, we architect a hierarchical microstructure integrating bimodal grain structures, nanoprecipitates, and hard-brittle coarse particles wrapped by ductility coarse grain (CG) bands via conventional cold rolling (CR) deformation and heat treatment methods to break the strength-ductility dilemma in the Al-8.89Zn-1.98Mg-2.06Cu-0.12Zr-0.05Sc-0.05Hf (wt.%) alloy. The results reveal that the coupling of high-volume fraction (∼1.2%) nanoprecipitates, ∼52% narrow CG bands, and most coarse particles encapsulated by CG bands contribute to the 45% CR sample with outstanding overall mechanical properties (a tensile strength of 655 MPa, a yield strength of 620 MPa, and an elongation of 15.5%). Microstructure-based strength analysis confirms that the high strength relates to a trade-off between the hierarchical features, namely high-volume fraction nanoprecipitates to counterbalance the strength loss caused by grain coarsening. The excellent ductility is due to the introduction of medium CG content with a narrow width that can trigger a cross-scale strain distribution during plastic deformation, suppressing the catastrophic failure in the fine grain (FG) regions and facilitating the dimple fracture along the CG bands. This study proposes a feasible approach for tailoring hierarchical microstructures in Al-Zn-Mg-Cu alloys to achieve a superior strength-ductility combination.