The mechanical properties and microstructure evolution of an Al-Cu-Li alloy sheet processed via hot rolling (HR) (at 400◦C and 500◦C) or cryorolling (CR) (at −100◦C and −190◦C) and subsequence aging at 160◦C for 10 h were investigated. Before aging, the highest ultimate tensile strength of 502 MPa was achieved when the sheets were cryorolled at −190◦C, while the better ultimate tensile strength of 476 MPa and the best elongation rate of 11.1% was achieved simulta-neously when the sheets were cryorolled at −100◦C. The refined grains and numerous uniform deformation-induced dislocations microstructures were responsible for the improved strength and enhanced ductility of the cryorolled sheets compared to that of the alloy processed by hot rolling with a low dislocation density zone (LDDZ) and high dislocation density zone (HDDZ). After aging at 160◦C for 10 h, the ultimate tensile strength further improved resulted from the greater precipitation strengthening, and the increased precipitates provided greater resistance to dislocations movement resulting in the increased ductility although the dislocation density decreased. The uniform dislocation microstructures in the cryorolled sheets provide numerous nucleation sites for the precipitates, leading to higher strength after aging.