Abstract: It is shown that order-disorder relations in the distribution of the isomorphous substitutions are important in the characterization of different 2/1 phyllosilicates and in the determination of their behavior. These order-disorder relations are shown by selected area diffraction patterns obtained from single crystals. The range of layer charges corresponding to smectites (charge per half-cell <0.6) is that for which phyllosilicates are stable with disordered substitutions. Phyllites with charge >0.6 show anomalous diffusions which indicate that the distributions of exchangeable Ba ions are partially ordered; this result is taken as evidence that the isomorphous substitutions also are partially ordered.