—Illite polytypes are used to elucidate the geological record of formations, such as the timing and provenance of deformations in geological structures and fluids, so the ability to characterize and identify them quantitatively is key. The purpose of the present study was to compare three X-ray powder diffraction (Q-XRPD) methods for illite polytype quantification for practical application to directly date clay-rich fault rocks and constrain the provenance of deformation-related fluids in clay-rich brittle rocks of the upper crust. The methods compared were WILDFIRE© (WF) modeling, End-member Standards Matching (STD), and Rietveld whole-pattern matching (BGMN®). Each technique was applied to a suite of synthetic mixtures of known composition as well as to a sample of natural clay gouge (i.e. the soft material between a vein wall and the solid vein). The analytical uncertainties achieved for these synthetic samples using WF modeling, STD, and Rietveld methods were ±4–5%, ±1%, and ±6%, respectively, with the caveat that the end-member clay mineral used for matching was the same mineral sample used in the test mixture. Various particle size fractions of the gouge were additionally investigated using transmission electron microscopy (TEM) to determine polytypes and laser particle size analysis to determine grain size distributions. The three analytical techniques produced similar 40Ar/39Ar authigenesis ages after unmixing, which indicated that any of the methods can be used to directly date the formation of fault-related authigenic illite. Descriptions were included for pre-calculated WF illite polytype diffractogram libraries, model end-members were fitted to experimental data using a least-squares algorithm, and mixing spreadsheet programs were used to match end-member natural reference samples.