We hope that the results of this study aid work where the calculation of large polarizability values is crucial. We note that for some applications, such as dielectric device development, the frequency dependence of polarizability should be considered, but is outside the scope of this work. While GFN2/D4 is not currently fit to provide accurate calculations for large polarizability values, we hope that after some minor corrections it will be a viable method for such applications and improve the accuracy of future dispersion correction methods. Considering the incredible e ciency, this would provide a valuable tool for future molecular screening studies of highly polarizable materials. Meanwhile, using lower-cost non-augmented basis sets with a correction factor vastly increases the number of potential molecular species for which highly accurate polarizabilities can be now obtained.