The fact that the NDDO/SMD errors are largest for ions suggest that the problem is with the polar solvation energy, so we focus on optimizing the values of the Coulomb radii while leaving all parameters associated with the non-polar solvation free energy unchanged. We optimize the radii only for the ionic species on a subset of the MNSOL data set previously used to parametrize RHF/6-31G(d)/SMD, but include neutral molecules when testing how well SMD with the new Coulomb radii perform. We found the best results are obtained by changing only the radii for hydrogen, carbon, oxygen, nitrogen, and sulfur and this leads to RMSE values for PM3 (neutrals: 2.8/ions: ca 5 kcal/mol), PM6 (4.7/ca 5 kcal/mol), and DFTB (3.9/ca 5 kcal/mol) that are more comparable to HF/6-31G(d) (2.4/ca 5 kcal/mol). We note that the SMD parameterization is done using mono-aquo microsolvated species for small ions with atoms carrying large (partial) charges, while the MNSOL data set also contains data for the non-microsolvated equivalents. Comparison to the HF/6-31G(d) MSEs reported by Marenich et al. reported for the selectively microsolvated ions indicates that the inclusion of non-microsolvated species leads an MSE increase of about 1 kcal/mol. Though the radii are optimized to reproduce aqueous solvation energies, they also lead more accurate predictions for other polar solvents such as DMSO, acetonitrile, and methanol, while the improvement for non-polar solvents are negligible.