Upon conclusion of the exploration stage, a final exploitation round, consisting of the acquisition of 30 points (with a β value of 1.0), was initiated. From this batch, the reaction profiles were successfully acquired for 26 reactions. The MAE of the predictions on this round was 0.61 kcal/mol, in line with the error obtained in the last exploration round, confirming that model convergence had indeed been reached. From the final pool of 108 acquired reactions, 70 were selected to form our new benchmarking dataset. A table containing the list of reactions for this new dataset organized by type, and the reference reaction energy and barrier heights can be found in Section S2.4 of the ESI. DLPNO-CCSD(T) reference values were computed for the acquired reactions (see Section S2.4 of the ESI for the methodology used), and the deviation for every functional was computed. The resulting accuracies are presented graphically in Figure , together with the accuracies for the original BH9 cycloaddition dataset (values are presented in Table of ESI).