Referring to SI table S1, when we examine the molecule with the largest error using OpenFF's default, B3LYP-D3(BJ)/DZVP, which exhibits an RMSE in relative energies of 1.36 kcal/mol, we observe that the majority of discrepancies arise from the high-energy region exceeding 5 kcal/mol. The torsion profile for this molecule with respect to different basis sets was shown in Figure . It is worth reiterating that we exclude this high-energy region during the training process.