Metavolcanic rocks of the Winterville Formation from the prehnite-analcime subfacies of the prehnite-pumpellyite facies in north-central Aroostook County, Maine, contain an alteration assemblage including chlorite, chlorite/smectite (C/S), analcime, prehnite, and calcite. Field and laboratory study has identified areas where hydrothermal alteration has been pervasive in and around pillows. Compositional, crystal chemical, and structural variations in chlorite appear to be related to distance from this hydrothermal alteration. Samples were studied by whole-rock chemical analysis, electron microprobe analysis of individual mineral grains, X-ray powder diffraction of the clay fraction, and by computer modeling of diffraction patterns to determine the percentage of chlorite in interstratified C/S and to estimate the distribution of Fe and the size of coherent diffracting domains in pure chlorites. Whole-rock and pyroxene compositions suggest that the rocks have undergone Mg metasomatism. Modeling of X-ray diffraction data indicates that the percentage of chlorite in C/S increases to 100%, that Fe atoms become more equally distributed between octahedral sites in chlorite as it becomes more Fe-rich, and that diffracting domains grow larger with proximity to areas of more intense hydrothermal alteration. Analcime also increases near areas of hydrothermal alteration. The areal distribution of hydrothermal effects suggests that the alteration occurred as two separate events, or that two different thermal regimes were active concurrently.