Abstract: In view of the unclear spatial distributions of sputtered atoms from ion engine grid, which leads to significant deviations in grid erosion modeling predictions, the SDTrimSP program was used to simulate the sputtering process of ions bombarding the grid materials. The study systematically investigated the impact of ion incident energy, incident angle, and ion species on the differential sputtering yields of molybdenum grid materials. Under normal incidence, the simulated differential sputtering yields were found to be in good agreement with experimental data. Special attention was given to the distribution profiles of differential sputtering yields at different azimuthal angles under oblique incidence. The Modified-Zhang formula was used to fit the differential sputtering yields. The fitting results were applied as material boundary conditions in the erosion-redeposition model, offering a more realistic simulation of the grid materials’ erosion process. This approach may provide a reference for the accurate prediction of the erosion morphology of ion engine grid components.