We presentN7VV(4f7/25d5d) Auger spectra from TaC(111) taken in time coincidence with photoemitted bulk and surface‐shifted 4f7/2core‐level electrons, and compare these data with self‐convolutions of calculated valence bandddensities of states (SCDOS) for the surface (first) and bulk (exponential sum of second, fourth, and sixth subsurface) atomic layers of a 13‐layer slab. The Ta 4flevels of TaC(111) and Ta(100) both exhibit large surface core level shifts, but of opposite sign. Therefore, we compare the TaC(111) data and calculations with analogousN7VVAuger coincidence spectra and calculated SCDOS that we have previously published for Ta(100). The bulk Ta(100) and surface TaC(111) spectra show favorable agreement with the calculations; the surface Ta(100) and bulk TaC(111) spectra, on the other hand, exhibit marked disagreement with the calculations. These discrepancies are consistent with and provide added support for the presence of our proposed1surface‐to‐bulk (bulk‐to‐surface) interatomic Auger decay mode which adds a bulk (surface) contribution to the surface (bulk) Auger line shape of Ta(100) (TaC(111)). These conclusions are supported by comparison of our data to incoherent sums of bulk and surface SCDOS.