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Notes: Abstract Illite crystallinity (IC) measurements, determination of the proportion of 2M mica-polytypes and organic-matter reflectance measurements establish regional diagenetic/low-grade metamorphic trends for the Taconian and Acadian belts of Gaspé Peninsula.IC varies as a function of many factors besides maximum burial temperature and heating time. Correlation between IC and %2M illite polytypes for the Fortin Group and Temiscouata Formation suggests (i) that the amount of high-grade detrital mica in the samples is low, and (ii) that IC can be used with some confidence as an estimator of regional thermal maturation levels. Correlation of these parameters with available organic reflectance values further supports this assumption. The illites of the Temiscouata and western Fortin groups are mostly phengitic in composition, whereas in the eastern outcrop belt they are more Mg- and Fe-rich (celadonitic), but generally also of lower grade and lower 2M content. The d(060) values for illites measured on the unorientated 〈2-μm fraction of samples fall between 1.502 and 1.503 Å (range: 1.500–1.504 Å), indicating relatively low octahedral occupancy by Mg and Fe (between one-fifth and one-third of the available spaces). Pyrophyllite and paragonite were not detected. Chlorites are Fe-rich and ripidolitic.The IC map for the Acadian belt of the peninsula displays general congruence between IC contours (2200 sample points) and structural trends for the 27,000-km2 area. The highest grades (anchimetamorphic) are associated with the oldest rocks (Honorat and Matapedia groups) exposed in the cores of major anticlines. Anchimetamorphic grades associated with the western outcrop belt of the Lower Devonian Fortin Group require 7–8 km of subsidence to accommodate sufficient thickness of overlying younger rocks (on top of 4–5 km of Fortin Group deep-water clastics) to explain the grades in terms of burial metamorphism assuming a geothermal gradient of 30° C km−1. The lowest-grade diagenetic rocks occupy a large area in the northeastern part of the peninsula, smaller areas in the northwestern part of the Acadian belt, in the centre of Chaleurs Bay synclinorium, and in the Ordovician Mictaw Group. The contact between the Taconian and Acadian belt is marked by a distinct maturation discontinuity. The Grand Pabos fault juxtaposes rocks of contrasting maturation levels (Matapedia Group against Fortin Group) in the west, but shows no maturation offset further east in the Honorat Group. The fault zone limiting the Fortin Group in the north is also associated with a major IC jump.