A newly recognized suite of trondhjemite–tonalite and dacitic gneiss forms a 10 km wide belt of rocks within the Mount Holly Complex in the central part of the Green Mountain massif of Vermont. Field relationships and chemistry indicate that these gneisses are calc-alkaline, volcanic, and hypabyssal plutonic rocks older than the Middle Proterozoic regional deformation that affected the Mount Holly Complex. U–Pb zircon dates indicate ages as great as 1.35 Ga for crystallization of the volcanic protoliths and for intrusion of crosscutting trondhjemite. Tonalitic plutonism continued until 1.31 Ga.Map-scale contacts between the trondhjemitic–tonalitic–dacitic gneisses and the paragneiss sequence of the Mount Holly Complex are sharp, suggesting that the volcanic rocks of the trondhjemite–tonalite suite underlie the paragneiss units and do not intrude them. These relationships suggest that the trondhjemite–tonalite suite is either considerably older than, and unconformable beneath, the paragneiss cover rocks or represents a volcanic edifice slightly older than the deposition of the sedimentary precursor to the paragneiss units. The paragneiss and tonalite–trondhjemite gneisses are both intruded by younger granitoids that were intruded at about 1.25 Ga during strong dynamothermal metamorphism.The trondhjemitic gneisses of the Mount Holly Complex of Vermont have high Al2O3 and low Yb contents and light rare-earth element enrichment patterns that are more characteristic of continental than oceanic volcanic arcs. The Mount Holly intrusives and volcanics may have formed during 1.35–1.31 Ga ensialic volcanic-arc activity, contemporaneous with ensimatic arc activity during the early part of the Elzevirian phase of the Grenville orogeny. In Vermont, later deformation and granite intrusion at about 1.25 Ga coincide with the major pulse of the Elzevirian orogeny and associated trondhjemitic plutonism in the Central Metasedimentary Belt of eastern Canada.