The presented work shows that a proper consideration of dynamics, temperature, explicit solvation, aluminium concentration and distribution is necessary to achieve a close agreement with experiment, and even allows for the assignment of Al NMR peaks in realistic model zeolites (such as MFI zeolite studied herein) under experimental conditions. We have reaffirmed some findings in the literature, such as the quantification of the role of Si/Al ratio, and we have dispelled some persistent inaccuracies, including the use of single structure models, the neglect of temperature and the use of averaged background charge models for high-water conditions.