We present major- and trace- element geochemical data for 27 amphibolites and six greenstones from three structural packages in the Yukon–Tanana Upland of east-central Alaska: the Lake George assemblage (LG) of Devono-Mississippian augen gneiss, quartz–mica schist, quartzite, and amphibolite; the Taylor Mountain assemblage (TM) of mafic schist and gneiss, marble, quartzite, and metachert; and the Seventymile terrane of greenstone, serpentinized peridotite, and Mississippian to Late Triassic metasedimentary rocks. Most LG amphibolites have relatively high Nb, TiO2, Zr, and light rare earth element contents, indicative of an alkalic to tholeiitic, within-plate basalt origin. The within-plate affinities of the LG amphibolites suggest that their basaltic parent magmas developed in an extensional setting and support a correlation of these metamorphosed continental-margin rocks with less metamorphosed counterparts across the Tintina fault in the Selwyn Basin of the Canadian Cordillera. TM amphibolites have a tholeiitic or calc-alkalic composition, low normalized abundances of Nb and Ta relative to Th and La, and Ti/V values of <20, all indicative of a volcanic-arc origin. Limited results from Seventymile greenstones indicate a tholeiitic or calc-alkalic composition and intermediate to high Ti/V values (27–48), consistent with either a within-plate or an ocean-floor basalt origin. Y–La–Nb proportions in both TM and Seventymile metabasalts indicate the proximity of the arc and marginal basin to continental crust. The arc geochemistry of TM amphibolites is consistent with a model in which the TM assemblage includes arc rocks generated above a west-dipping subduction zone outboard of the North American continental margin in mid-Paleozoic through Triassic time. The ocean-floor or within-plate basalt geochemistry of the Seventymile greenstones supports the correlation of the Seventymile terrane with the Slide Mountain terrane in Canada and the hypothesis that these oceanic rocks originated in a basin between the continental margin and an arc to the west.