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The Tyrone Igneous Complex is one of the largest areas of ophiolitic and arc-related rocks exposed along the northern margin of Iapetus within the British and Irish Caledonides. New U–Pb zircon data and regional geochemistry suggest that the Tyrone Plutonic Group represents the uppermost portions of a c. 480 Ma suprasubduction-zone ophiolite accreted onto an outboard segment of Laurentia prior to 470.3 ± 1.9 Ma. The overlying Tyrone Volcanic Group formed as an island arc that collided with the Laurentian margin during the Grampian phase of the Caledonidan orogeny. Early magmatism is characterized by transitional to calc-alkaline, light REE (LREE)-enriched island-arc signatures, with an increasing component of continentally derived material up sequence. Tholeiitic rhyolites with flat to U-shaped REE profiles and LREE-depleted basalts, located stratigraphically below a c. 473 Ma rhyolite of the upper Tyrone Volcanic Group, suggest initiation of intra-arc rifting at c. 475 Ma. Metamorphic cooling ages from the Tyrone Central Inlier imply arc–continent collision before 468 ± 1.4 Ma, with the emplacement of the Tyrone Volcanic Group onto the margin. A suite of 470.3 ± 1.9 Ma to 464.3 ± 1.5 Ma calc-alkaline intrusions are associated with the continued closure of Iapetus.