The addition of oversized solutes has the potential to reduce the effects of radiation-induced segregation (RIS) in austenitic alloys. This RIS has been implicated as one of several factors in enhancing stress corrosion cracking (SCC) under irradiation, so oversized solute additions could promote SCC resistance. Either Zr or Hf was added to 316-type stainless steel, at levels between 0.05 and 0.37 at. pct. Samples were irradiated with 3 MeV protons to 3 dpa at 400°C and analyzed using high-resolution-scanning transmission electron microscopy (HR-STEM) with energy-dispersive X-ray spectroscopy (EDS), to measure the grain-boundary (GB) composition. The Zr additions substantially reduced the amount of RIS, while the Hf was much less effective. Despite similar sizes, first-principles calculations using the Vienna Ab Initio Simulation Package (VASP) demonstrate that solute-vacancy binding for Zr is 1.05 eV vs 0.69 eV for Hf. This difference results in the greater effectiveness of Zr in reducing RIS, as determined by kinetic rate theory calculations, in agreement with experimentally-measured results.