For samples with a sufficiently high Si/Al ratio, we show that even for MFI (ZSM-5) zeolite, one might be able to reliably assign NMR peaks to specific T-sites if realistic models are adopted, achieving almost quantitative agreement between the experimentally and computationally predicted range of NMR peaks and their positions. Indeed, given the quantitative agreement obtained, the increased range of measured NMR resonances might be used as an indication of the formation of the Al pairs and Al zoning. Clearly, one has to be cautious not to over-interpret the tentative assignments, which is unfortunately not uncommon in the field -for instance, within a narrow, 3 ppm range, signals for 16 different Tsites are expected, leading to significant overlap. Hence, achieving a definitive assignment of calculated chemical shifts to experimental peaks is challenging and to overcome this limitation, e.g., additional NMR parameters (such as chemical shift anisotropy) will be necessary to extract more detailed information from the NMR spectrum.