Chemical analyses of sixteen lithium-aluminium micas are presented along with their optical, physical, and X-ray data. Compositional variation, substitution relations in structural positions, and octahedral occupancy are discussed. The 2M₂ structural types are found to crystallize in volatilerich low-temperature environments whereas the 1M polytypes occur in comparatively volatile-poor and higher-temperature environments. Variation diagrams have been constructed to show the relationship between octahedral sites occupied by (Fe²⁺+ Fe³⁺+13Mn+Ti) and refractive indices and specific gravities.