This study aims to model the effects of multiple laser peening (LP) on the mechanical properties of AA2024-T351 by including the material microstructure and residual stresses using the crystal plasticity finite element method (CPFEM). In this approach, the LP-induced compressive residual stress distribution is modeled through the insertion of the Eigenstrains as a function of depth, which is calibrated by the X-ray measured residual stresses. The simulated enhancement in the tensile properties after LP, caused by the formation of a near-surface work-hardened layer, fits the experimentally obtained tensile curves. The model calculated fatigue indicator parameters (FIPs) under the following cyclic loading application show a decrease in the near-surface driving forces for the crystal slip deformation after the insertion of the Eigenstrains. This leads to a higher high cycle fatigue (HCF) resistance and the possible transformation of sensitive locations for fatigue failure further to the depth after LP. Experimental observations on the enhancement in the HCF life, along with the relocation of fatigue crack nucleation sites further to the depth, reveal the improvement in the HCF properties due to the LP process and validate the numerical approach.