It turns out that regularization in κDSD-PBEP86-D3BJ becomes gradually more beneficial as cX,HF is decreased, with κmin decreasing concomitantly. For example, we obtain the lowest WTMAD2 near κ=1.67 when cX,HF=0.55, but when cX,HF=0.5 is used, the κmin drops to 1.45 (see Figure ). Now, splitting each WTMAD2 into five major subcategories, we found that regularization does more harm than good across the board for small-molecule thermochemistry. However, the extent of performance deterioration with respect to the κ values becomes less prominent as cX,HF in κDSD-PBEP86-D3BJ is reduced. Using a small κ value can severely harm the performance for barrier heights at elevated percentages of HF exchange, but much less so at lower percentages. At κ=1.1, the κDSD50-PBEP86-D3BJ marginally outperforms the unregularized variant. For large-molecule reactions, κDSD-PBEP86-D3BJ is a better choice across the board compared to the revDSD-PBEP86-DBJ functional, and κmin decreases gradually with the increase of cX,HF. The κDSD69-PBEP86-D3BJ and κDSD66-PBEP86-D3BJ functionals offer the best performance near κ=3.0 and 2.0, respectively. With κ=1.45, the ΔWTMAD2 (i.e., the contribution from a particular subset for total WTMAD2) for κDSD55-PBEP86-D3BJ is very close to what we obtained for the unregularized functional form. For intramolecular interactions, the trends are largely the same as what we obtained for the small-molecule thermochemistry subsets. Finally, for intermolecular interactions, regularized forms always outperform the unregularized alternatives, and κmin decreases with increasing of cX,HF. For this subset κDSD69-PBEP86-D3BJ and κDSD63-PBEP86-D3BJ are the two best picks at κ=1.45 and 1.33, respectively. (For optimized parameters, total WTMAD2 for full GMTKN55, and its decomposition into five major subsets see Table in the Supporting Information.)