Pre-deformation is usually indispensable to obtain an appropriate balance between microstructure and mechanical properties of Al-Cu-Li alloys. In this paper, the effect of pre-deformation degree on the evolution of strength, fracture toughness, and precipitates during artificial aging processes of a novel Al-Cu-Li alloy was studied. The results indicated that the amount of T1 phase increased remarkably while the precipitation of θ' phase was inhibited with the increase of pre-deformation degree. The change in the average size of T1 phase indicated that the increase in nucleation sites suppressed the full growth of T1 phases. The fracture toughness could be related to the strength difference between intragranular and intergranular. Based on the matching of properties, a reasonable pre-deformation parameter was proposed.