Aiming to improve the mechanical properties and fatigue performance of 2024 aluminum alloy, the experimental investigations on composite treatment consisting of ultrasonic shot peening (USP) followed by surface mechanical rolling (SMR) were carried out. The experimental results were compared with the specimens only treated by USP or SMR in terms of surface roughness, microhardness gradient and microstructure observation. The uniaxial tension test and low cycle fatigue test were conducted on the as-received specimen and the ones treated by USP, SMR and USP/SMR composite treatment, respectively. The tensile mechanical properties were effectively improved by USP. The introduction of SMR following USP can significantly increase the number of cycles to failure. Combining fracture morphology analysis and DEM-FEM coupling simulation of USP/SMR composite treatment, it was concluded that the improvement of tensile mechanical properties is mainly attributed to the synergistic effect of the compressive residual stresses and gradient-structured layer produced by USP, and the decrease in surface roughness resulting from SMR is the main reason for the significant improvement of fatigue performance. This work could provide an insight into the surface strengthening mechanism for USP/SMR composite treatment of materials with respect to the improvement of mechanical properties and fatigue performance.