In order to further enhance the strength and ductility of ultra-high strength aluminum alloys, the laser shock peening technology was applied to ultra-high strength Al-Zn-Mg-Cu alloy. The ultimate tensile strength, elongation and hardness can reach to 751 MPa, 11 % and 208.3 HV by combining spray forming, secondary extrusion, solid solution, retrogression and reaging as well as laser shock peening. The high strength and hardness of the alloys is mainly attributed to the fine-grained layer on surface as well as new grain boundaries, dislocation cells and high-density dislocations introduced by laser shock peening, uniform nano-sized strengthening phases with high density precipitated during heat treatments. The excellent ductility of the alloys is mainly ascribed to multiple structures including fine-grained layer on surface and slip lines inside different grains introduced by laser shock peening, smaller size of fibrous grains and Al7Cu2Fe phase produced by secondary extrusion and spray forming. The aging treatment after laser shock peening can lead to the annihilation of high-density dislocations as well as significantly promote the formation of stable and coarse η phase, which can greatly reduce the strength of the studied alloys.