Textural and chemical changes occurring in illite and chlorite concomitant with pressure solution of limestone were studied in samples from the Kalkberg Formation of Catskill, New York, using XRD and TEM/AEM. Samples on one limb of an anticline are massive shaly limestones, but those on the other have undergone extensive pressure solution and well-developed cleavage is present. Illite and chlorite from the uncleaved shaly limestone are found in small individual packets (100–800 Å thick) dispersed throughout the carbonate matrix with crystal morphologies characteristic of burial diagenesis. Phyllosilicates from the limb more affected by pressure solution occur in larger units (>1 μm thick) as stacks of subparallel packets (150–500 Å thick). Such stacks are inferred to represent coalescence of smaller packets. These data imply that the phyllosilicates are largely passive during pressure solution of limestone; however, localized solution-recrystallization is required by the coherent to semi-coherent packet boundaries and the crystal morphologies present in the pressure solution sample. The largely passive role is in contrast with the more active role of phyllosilicates in many shales and slates. XRD data for illite show an increase in crystallinity in the pressure solution sample under isothermal conditions. Differences in illite crystallinity are adequately explained in large part by differences in crystal size with some contribution due to strain. The data demonstrate that illite crystallinity cannot be unambiguously used in determining absolute or even relative temperatures.