This study evaluated the feasibility of using STEM-EELS to measure coordination changes of Al in kaolinite upon calcination; and its potential applicability to determine Al coordination changes in Fe-rich kaolinitic clays. The approach of this study was to use 27 Al MAS NMR measurements on a low-Fe clay to benchmark the use of EELS for this mineral system, and then to use STEM-EELS on an Fe-rich clay to assess the change in kaolinite Al co-ordination induced by calcination.