New Al-4.5Cu-1Li-0.7Mg-1Zn-0.3Ag-0.3Mn-0.2Zr aluminium lithium alloys were prepared by casting and hot formation. The effects of cold-rolled pre-deformation on microstructure and mechanical properties after solid solution were investigated using Vickers hardness, tensile testing, scanning electron microscopy and transmission electron microscopy. The results show that cold-rolled pre-deformation can effectively promote the precipitation of T1 phases and reduce the volume fraction of θ" phases in the matrix. Adding cold-rolled pre-deformation resulted in an enhanced age hardening response and shorter the time to reach peak aging. At the same time, the grain boundary precipitates change from continuous precipitation to discontinuous precipitation, and the width of the PFZs becomes smaller. The yield strength, tensile strength and elongation of as-aged alloy, when the pre-deformation amount was 15%, were 668 MPa, 690 MPa and 7.9%, respectively.