During the preparation of the manuscript, we inadvertently made two mistakes: (1) We used aqueous solvation free energy of proton for pKa calculations in acetonitrile, and (2) in the comparison between the accuracy of SMD, our revised CPCM-UAHF and COSMO-RS, we forgot to use the keyword radii = klamt in generating cosmo files of 11 ions in water. Thus, several figures and tables need to be changed; however, the conclusions reached in the Article remain unchanged. 1. Correction to pKa Values in Acetonitrile. We inadvertently used the aqueous solvation free energy of proton in pKa calculations in acetonitrile in the original version. Here we recalculate all pKas in acetonitrile using the experimental value of the solvation free energy of proton as −260.2 kcal/mol as taken from ref (1). All calculated pKa values in tab “pKa calculations” in our original Supporting Information have been corrected; see the corrected Supporting Information. It can be seen that the accuracy of pKa calculations in acetonitrile reported previously is underestimated. When using the correct solvation free energy of the proton in acetonitrile, our calculated pKa results are much improved compared that reported previously. Figures 3 and 5 and Supporting Information Tables S11 and S12 have been changed. Figure 1. Mean absolute errors (MAEs) of solvation Gibbs free energies of neutral and ionic solutes calculated with different solvation models. Figure 3. Mean absolute errors (MAEs) in the nonaqueous (acetonitrile) pKa values of Scheme 2, as calculated using mixed ESF values. pKa values of solute types labeled in red (PYR1–PYR5) are calculated with cations and neutrals, while those in blue are calculated with neutrals and anions. For all other computations, see Computational Details. Figure 5. Mean absolute errors (MAEs) of 20 pKa calculations in acetonitrile obtained with different ESF combinations using the IEFPCM-UAKS method. For example, 1-0-3 means using ESF = 1.1, 1.0, and 1.3, respectively, for neutrals, cations, and anions. In our original work, based on the results in the original Figure 5, we concluded the optimal ESF value of neutrals in acetonitrile might need a slight change. While here, 2-1-4 gives the smallest overall MAE, which proves using the ESF values obtained from our benchmarking gives the best results among all possible ESF combinations and does not need further change. 2. Correction to COSMO-RS Solvation Free Energies of Ions in Water. In the comparison between the accuracy of SMD, our revised CPCM-UAHF and COSMO-RS, we inadvertently forgot to use the keyword radii = klamt in generating cosmo files of the 11 ions in water, which makes the error of COSMO-RS quite large. Related data in the “CPCM-UAHF VS SMD VS COSMO-RS” tab in the Supporting Information and Figure 1 in the main text need to be changed. Note that only COSMO-RS solvation free energies of ions in water need to be changed, and based on the new results, our revised CPCM-UAHF model still outperforms COSMO-RS but not SMD, thus the main conclusion and discussion in comparing these three solvation models in our original paper does not change. The “CPCM-UAHF VS SMD VS COSMO-RS” tab in the Supporting Information now contains the correct solvation free energies of 11 ions. Thus, in Figure 1 of the publication, the mean absolute error of the COSMO-RS solvation free energies of ions should be 8.36 kcal/mol, and that of all 82 solute/solvent combinations should be 2.36 kcal/mol. The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.jctc.9b01191. Detailed data of ESF benchmarking, comparison between CPCM-UAHF, SMD, and COSMO-RS; calculation results at ωB97X-D/6-31+G(d,p) theoretical level (XLSX) Main results of ESF benchmarking; raw data of pKa calculations; optimized structures of 65 molecules (PDF) Detailed data of ESF benchmarking, comparison between CPCM-UAHF, SMD, and COSMO-RS; calculation results at ωB97X-D/6-31+G(d,p) theoretical level (XLSX) Main results of ESF benchmarking; raw data of pKa calculations; optimized structures of 65 molecules (PDF) Electronic Supporting Information files are available without a subscription to ACS Web Editions. The American Chemical Society holds a copyright ownership interest in any copyrightable Supporting Information. Files available from the ACS website may be downloaded for personal use only. Users are not otherwise permitted to reproduce, republish, redistribute, or sell any Supporting Information from the ACS website, either in whole or in part, in either machine-readable form or any other form without permission from the American Chemical Society. For permission to reproduce, republish and redistribute this material, requesters must process their own requests via the RightsLink permission system. Information about how to use the RightsLink permission system can be found at http://pubs.acs.org/page/copyright/permissions.html. This article references 1 other publications.