To probe the effect of water loading as well as obtain the values of Al NMR chemical shifts in MFI under realistic hydrated conditions we considered the following water loadings: 0, 1, 2, 3, and 17 water molecules per unit cell. The model of 17 water molecules is expected to correspond to fully hydrated zeolite at ambient conditions, as justified by the experimental measurements of Holzinger et al. , who reported 15 ± 1 water molecules per unit cell present for H-ZSM-5 with a Si/Al ratio of 50. These water loadings were probed for MFI models with one aluminium atom per unit cell (Si/Al = 95) and all crystallographically inequivalent T-sites in MFI (12 T-sites) were considered. In addition, various initial BAS configurations in the vicinity of each T-site were considered (see details in the Section S6 †).