The Dover Fault forms a tectonic boundary between northern portions of the Gander and Avalon Zones of the Newfoundland Appalachians. A systematic geochronological investigation across the mylonitic fault zone has been carried out to clarify the origin and history of tectonic activity along this important Appalachian structure.Zircon fractions from the mylonitic Lockers Bay Granite (Gander Zone) record individually discordant U–Pb dates, but yield a well-defined upper concordia intercept age of 460 ± 20 Ma. Hornblende (1 sample) and biotite (11 samples) from variably mylonitic Gander Zone lithologies (plutonic and metamorphic) adjacent to the fault zone record undisturbed 40Ar/39Ar age spectra with plateau ages of 395 and 365–383 Ma, respectively. Together with field and petrographic characteristics, the new geochronologic data suggest that the Lockers Bay Granite originated as an anatectic melt during high-grade regional metamorphism of the country rock terrane at approximately 460 Ma. The crystal-rich magma was subsequently emplaced into its present position thereby producing local discordance with small-scale structures in host gneisses.Following its emplacement, the Lockers Bay Granite and country rock terrane were maintained at elevated postmetamorphic temperatures for a prolonged interval until they underwent rapid strain during Acadian (Devonian) juxtaposing of the northern Gander and Avalon Zones along the Dover Fault. Sudden Acadian uplift along the fault is suggested because of the rapid cooling of the northern Gander Zone through temperatures required for argon retention in hornblende and biotite. Post-mylonite brecciation may have locally affected argon isotopic systems of phyllitic lithologies adjacent to the fault zone in the study area.