Magic angle spinning nuclear magnetic resonance (MAS NMR) spectroscopy is typically used to explore changes in Al coordination after calcination . Using appropriate models that account for quadrupolar broadening, e.g. the Czjzek model , it is possible to deconvolute 27 Al MAS NMR spectra and hence obtain quantitative measurements of the proportions of sites in each coordination state . When applied to as-received kaolinite, there is a general consensus that nearly all Al sites are in 6-fold coordination. If calcined at high temperatures sufficient to cause re-crystallisation (typically above 900°C), nearly all Al sites are in 4-fold coordination. In meta-kaolinite, 27 Al MAS NMR spectra exhibit three distinct resonances, with a distribution of Al sites in broadly similar proportions -typically assigned to 4-fold, 5-fold and 6fold co-ordination states . However, the assignment of the mid-range resonance as 5-fold Al is contestedan alternative interpretation is 4-fold Al coordination in a highly disordered local environment, wherein the disorder causes a substantial deviation in chemical shift from the expected range for 4-fold Al in aluminosilicates . There is further debate around 6-fold Al in meta-kaolinite. Studies consistently report a 27 Al MAS NMR substantial resonance associated with 6-fold Al in meta-kaolinite's 27 Al MAS NMR spectrum , yet structural models developed from neutron scattering yield no 6-fold Al remaining at all . Given that a detailed scientific understanding of meta-kaolinite's structure and the dehydroxylation process itself is not yet complete, additional characterisation techniques have value in bringing new perspectives to these fundamental questions.