Devonian–Mississippian felsic rocks from the Finlayson Lake region have variable geochemical and Nd isotopic characteristics that provide insights into the tectonic and metallogenic evolution of the Yukon–Tanana terrane (YTT), and the northern Cordillera. Late Devonian (∼365–360 Ma) calc-alkaline and tholeiitic arc felsic rocks in the mafic-dominated Fire Lake unit yield εNd350 = –4.8 and +0.1, respectively, and have 1.49–1.94 Ga depleted mantle model ages (TDM). Devonian–Mississippian (∼360–356 Ma) felsic volcanic (Kudz Ze Kayah unit, Wolverine succession) and intrusive rocks (Grass Lakes suite) associated with volcanogenic massive sulphide (VMS) deposits have εNd350 = –7.8 to –9.5 with TDM = 1.59–2.25 Ga. A granitoid sample from the Early Mississippian (∼350–345 Ma) Simpson Range plutonic suite has εNd350 = –12.9 and TDM = 2.01 Ga, similar to previously reported values for this suite. The VMS-associated Grass Lakes suite of granitoids has higher high field strength element (HFSE) and rare-earth element (REE) contents, and higher Zr/Sc, Zr/TiO2, Nb/La, and Zr/La values relative to the Simpson Range plutonic suite; these geochemical features are similar to coeval VMS-associated felsic volcanic rocks in the Kudz Ze Kayah unit. The identification of similar HFSE–REE-enriched felsic volcanic and subvolcanic intrusive rocks may aid in delineating prospective regions for VMS mineralization in the YTT and other continental-margin arc to back-arc environments. The geochemical and Nd isotopic data for these YTT felsic rocks suggest that they reflect episodic mid-Paleozoic arc (Fire Lake unit; Simpson Range plutonic suite) and back-arc magmatism (Kudz Ze Kudz unit; Wolverine succession) built upon a transitional basement with variable, but significant, influence from evolved (Proterozoic) crustal materials.