A more rigorous theoretical treatment of methods previously used to correlate computed energy values with experimental redox potentials, combined with the availability of well-developed computational solvation methods, results in a shift away from computing ionization potentials/electron affinities in favor of computing absolute reduction potentials. Seventy-nine literature redox potentials measured under comparable conditions from 51 alternant and nonalternant polycyclic aromatic hydrocarbons are linearly correlated with their absolute reduction potentials computed by density functional theory (B3LYP/6-31+G(d)) with SMD/IEF-PCM solvation. The resulting correlation is very strong (R(2) = 0.9981, MAD = 0.056 eV). When extrapolated to the x-intercept, the correlation results in an estimate of 5.17 ± 0.01 eV for the absolute potential of the ferrocene-ferrocenium redox couple in acetonitrile at 25 °C, indicating that this simple method can be used reliably for both calculating absolute redox potentials and for predicting relative redox potentials. When oxidation and reduction data are evaluated separately, the overall MAD value is improved by 50% to 0.028 eV, which improves relative potential predictions, but the computed values do not extrapolate to a reasonable estimate of the absolute potential of the ferrocene-ferrocenium ion reference.