The MudMaster computer program, based on the modified Bertaut-Warren-Averbach (BWA) XRD method, was used in the study of diagenetic evolution of illitic material in shales. The illitic material was characterized by XRD as a mixture of illite-smectite (I-S) and discrete illite. The experimental conditions for complete dehydration of swelling clays, necessary in this method, were established for a climate of high relative humidity (RH >40%). It was found that the distribution of crystallite thickness of dehydrated illitic material of shales is described by the lognormal law, as was established earlier by the BWA method for pure I-S from pyroclastic rocks. The parameters characterizing this distribution evolve with depth: the mean crystallite thickness (Te), the distribution broadening (DW) and the parameter of a lognormal distribution (β2) increase, whereas the percentage of the most frequent crystallite thickness decreases. The observed scatter of values is not random but indicates fluctuations in the characteristics of the illitic material of shales. The results imply that the modified Scherrer technique of measuring mean crystal thickness from the broadening of XRD reflections can be extended at least to some shales.