Abstract: A ternary plot of the tetrahedral R3+ and octahedral R3+ populations for the dioctahedral 2:1 clay minerals shows a broad range of compositional variation within each of the major clay minerals. The clay minerals can be subdivided on the basis of total charge, location of the charge, and the relative amounts of Al and Fe3+ in the octahedral sheet. The division is natural and is controlled by the misfit between the tetrahedral and octahedral sheets and the need for tetrahedral rotation. The compositions of the tetrahedral and octahedral sheets are interdependent. Whereas muscovite has a lower limit of 1·7 Al octahedral occupancy, illite and montmorillonite have a lower limit of 1·3 Al; lower Al values result in the formation of a chain structure.