The Avalon Zone hosts well-preserved examples of high- and low-sulfidation epithermal Au-Ag mineralization and associated phyllosilicate alteration. Using examples from the Hope Brook and Hickey's Pond high-sulfidation systems (HSS) and the Heritage low-sulfidation system (LSS), this study presents new data on the mineralogical and chemical characterization of phyllosilicates associated with epithermal Au-Ag deposits. Electron probe microanalysis and X-ray diffraction studies revealed that the HSS examples contain Fe muscovite ((K0.62–0.79Na0.10–0.37Ca0.00–0.01)Al1.31–1.72(Mg0.01–0.08Fe0.05–0.19)(Al1.00–1.24Si2.76–3.00O10)(OH)2), paragonite ((K0.05–0.30Na0.78–1.02Ca0.00–0.01)Al1.66–1.84(Mg0.00–0.01Fe0.02–0.04)(Al1.01–1.11Si2.89–2.99O10)(OH)2), Al clinochlore ((Mg2.42–2.65Fe1.62–1.78)(Si2.57–2.69Al1.31–1.43O10)(OH)8), pyrophyllite, kaolin minerals, illite-smectite (I-Sme) and chlorite-smectite (C-Sme). Conversely, the LSS examples contain Fe-Mg muscovite ((K0.44–0.76Na0.00–0.02Ca0.00–0.01)Al1.55–1.82(Mg0.17–0.31Fe0.05–0.12)(Al0.55–0.71Si3.29–3.45O10)(OH)2), Al clinochlore ((Mg2.17–2.56Fe1.59–2.01)(Si2.71–2.92Al1.08–1.29O10)(OH)8), and I-Sme and C-Sme intermediates. Chlorite geothermometry indicated that HSS and LSS assemblages crystallized at average temperatures of 261 °C and 145 °C, respectively. Mica and chlorite from HSS and LSS are defined by Tschermak substitution and high-temperature polytypism (2M1 and IIb, respectively). In the HSS examples, one or more pulses of hot, acidic fluid reacted with host rocks generating an envelope of advanced argillic alteration (Fe-Ms, Kln, Pg, Prl) around a vuggy silica core. This is bounded by a zone of argillic alteration (Fe-Ms, Kln), with sericitic/chloritic alterations (Fe-Ms, Al-Clc) developed in distal parts of the systems. In the LSS, near-neutral hydrothermal fluids led to the formation of broad phyllic/chloritic zones (Fe-Mg Ms and Al-Clc). A low temperature overprint with 1M mica, Ib clinochlore ((Mg2.48–2.74Fe1.58–1.73)(Si3.05–3.15Al0.85–0.95O10)(OH)8), kaolinite and Sme-poor I-Sme and C-Sme is attributed to late waning stage hydrothermal activity and/or weathering. A close paragenetic link was established between Fe-Mg muscovite and Ag mineralization at Heritage, as well as between Fe-Mg muscovite and bladed calcite, suggesting boiling as the precipitation mechanism. The present study provides guidance on how phyllosilicate assemblages have the potential to discern HSS versus LSS mineralization during early prospection in terranes with limited exposure, and to contribute to the reconstruction of their hydrothermal record.