The Green Mountain Formation of early Proterozoic age in the Sierra Madre Range of southeastern Wyoming comprises a bimodal mafic and felsic volcanic assemblage. The rocks, which are chiefly breccias, agglomerates, flows, and volcaniclastic sediments, represent both subaerial and submarine eruptions and in part were redeposited in fluvial and nearshore marine environments. Volcanic rocks are clearly calc-alkaline in character and share a large number of geochemical features in common with continental-margin arcs or evolved oceanic-arc systems.The low Mg numbers and Ni contents of the basalts require 30–40% olivine fractional crystallization, and the high contents of the most incompatible elements, high (La/Sm)N ratios, and low Zr/Nb ratios require an undepleted or enriched mantle source. Geochemical data are consistent with an origin for the felsic volcanics and associated Encampment River granodiorite by shallow fractional crystallization of calc-alkaline basalt in a tectonic setting similar to modern arc systems. The near absence of andesites may reflect the retention of andesitic magma in crustal reservoirs during fractional cyrstallization.