To decide which of the methods introduced in Section 2.6 (Lippmaa's approximation, 2p-LASSO, 5p-LASSO, and KRR) to adopt for calculation of chemical shifts, we first benchmark their perfor-mance. The 2p-LASSO, 5p-LASSO, and KRR models were trained on the original database from Lei et al., containing aluminium atoms in a tetrahedral configuration within the MOR and CHA zeolites, varying in water content and Si/Al ratios. To compare their prediction accuracy, we generated a new testing set composed of a set of structures from NNP-driven MD simulations of MFI zeolites with Si/Al ratio of 95 and with five different water loadings (0, 1, 2, 3, and 17 water molecules per unit cell). For each water loading, two BAS configurations were chosen. The selected initial BAS configurations, as well as details of the procedure are provided in Section S4 †. Ten structures were sampled from each of these models (different water loading and BAS configurations, i.e., a hundred structures in total), and the chemical shifts were calculated using each method. These predicted values were then compared with the reference DFT chemical shifts, and the mean absolute error (MAE) was calculated to assess the accuracy of each method.