Among the enormously abundant natural occurrences of clay minerals, many examples are encountered in which no single specific crystallization scheme extends through a single ultimate grain. The characterization of such assemblages becomes an analysis of the distribution of matter within such grains, rather than the simple identification of mineral species. It having become established that the particular coordination complex typified by mica is a common component of many natural subcrystalline assemblages, the opportunity is afforded to analyze scattering from random associations of these complexes with other structural units. Successful analyses have been made of mixed hydration states of montmorillonite, of montmorillonite with mica, of vermiculite with mica, and of montmorillonite with chlorite, all of which are variants of the mica complex, and of halloysite with hydrated halloysite.