AbstractMuch emphasis has been placed recently on the role of Ostwald-type processes (both ripening and the step rule) in the formation of interstratified illite-smectite clay minerals during diagenesis. Closer investigation of the relationships between illite particle thickness (as defined in terms of the fundamental particle theory) and particle chemistry show that simple Ostwald ripening is too simplistic a mechanism to describe observed changes in illite thickness and composition. In addition, available thermodynamic data on clay minerals suggest that the conventional notion of metastability associated with Ostwald's step rule is an inaccurate description of the relationship between illitic clay minerals and their macroscopic 2 : 1 phyllosilicate analogues.