Exposed in the Machias-Eastport area of southeastern Maine is the thickest (at least 8,000 m), best exposed, best dated, and most nearly complete succession of Silurian and Lower Devonian volcanic strata in the coastal volcanic belt, remnants of which crop out along the coasts of southern New Brunswick, Canada, and southeastern New England in the United States. The volcanics were erupted through the 600-700-million-year-old Avalonian sialic basement. To test the possibility that this volcanic belt was a magmatic arc above a subduction zone prior to presumed Acadian continental collision, samples representing the entire section in the Machias-Eastport area of Maine were chemically analyzed. Three strongly bimodal assemblages of volcanic rocks and associated intrusives are recognized, herein called the Silurian, older Devonian, and younger Devonian assemblages. The Silurian assemblage contains typically nonporphyritic high-alumina tholeiitic basalts, basaltic andesites, and diabase of continental characterand calc-alkalic rhyolites, silicic dacites, and one known dike of andesite. These rocks are associated with fossiliferous, predominantly marine strata of the Quoddy, Dennys, and Edmunds Formations, and the Leighton Formation of the Pembroke Group (the stratigraphic rank of both is revised herein for the Machias-Eastport area), all of Silurian age. The shallow marine Hersey Formation (stratigraphic rank also revised herein) of the Pembroke Group, of latest Silurian age (and possibly earliest Devonian, as suggested by an ostracode fauna), contains no known volcanics; and it evidently was deposited during a volcanic hiatus that immediately preceded emergence of the coastal volcanic belt and the eruption of the older Devonian assemblage. The older Devonian assemblage, in the lagoonal to subaerial Lower Devonian Eastport Formation, contains tholeiitic basalts and basaltic andesites, typically with abundant plagioclase phenocrysts and typically richer in iron and titanium and poorer in magnesium and nickel than the Silurian basalts; and the Eastport Formation has rhyolites and silicic dacites that have higher average SiO2 and K2O contents and higher ratios of FeO* to MgO than the Silurian ones. The younger Devonian assemblage is represented by one sample of basalt from a flow in red beds of the post-Acadian Upper Devonian Perry Formation, and by three samples from pre-Acadian diabases that intrude the Leighton and Hersey Formations. These rocks are even richer in titanium and iron and poorer in magnesium and nickel than the older Devonian basalts. Post-Acadian granitic plutons exposed along the coastal belt for which analyses are available are tentatively included in the younger Devonian assemblage. The most conspicuous features of the coastal volcanics and associated intrusives are the preponderance of rocks of basaltic composition ( < 52 percent SiO2 ) in the Silurian assemblage, and the near absence in all assemblages of intermediate rocks having 57-67 percent SiO2 (calculated without volatiles). All the rocks are variably altered spilites and keratophyres. The basaltic types are adequately defined, however, by eight samples of least altered basalts having calcic plagioclase, clinopyroxene, and 0.5 percent or less CO2 , The more altered basalts are variably enriched or depleted in Na2O, K2O, and CaO relative to the least altered ones. In the silicic rocks no primary ferromagnesian minerals are preserved. The Na2O and K2O contents of the silicic rocks are erratic; they are approximately reciprocal, possibly owing to alkali exchange while the rocks were still glassy. We propose that the coastal volcanic belt extended along an axis of thermal swelling in the Earth's mantle and upward intrusion of partially melted mantle into the sialic Avalonian crust. These processes were accompanied by shoaling and emergence of the belt, and they produced the bimodal volcanism. Tholeiitic basaltic melts segregated from mantle material