Global maps of crustal thickness on the Moon, derived from gravity measurements obtained by NASA’s Gravity Recovery and Interior Laboratory (GRAIL) mission, have shown that the lunar crust is thinner than previously thought. Hyperspectral data obtained by the Kaguya mission have also documented areas rich in olivine that have been interpreted as material excavated from the mantle by some of the largest lunar impact events. Numerical simulations were performed with the iSALE-2D hydrocode to investigate the conditions under which mantle material may have been excavated during large impact events and where such material should be found. The results show that excavation of the mantle could have occurred during formation of the several largest impact basins. Even though large areas in the central portions of these basins were later covered by mare basaltic lava flows, surficial lunar mantle deposits are predicted in areas external to these maria. Our results support the interpretation that the high olivine abundances detected by the Kaguya spacecraft could indeed be derived from the lunar mantle.