The Coastal Complex (CC) and Bay of Islands Complex (BOIC) represent two supra-subduction zone (SSZ) forearc ophiolitic assemblages of different ages within the Taconic Humber Arm Allochthon of the Western Newfoundland Appalachians. To further constrain age relationships between the CC and BOIC and earliest initiation of Iapetus subduction, we acquired LA-ICP-MS U-Pb zircon ages for eleven plagiogranites sampled along strike of the CC belt. These ages combined with three prior legacy ages establish an age range of 514.3–502.7 Ma for the six CC plagiogranite plutons. The oldest precise ca. 514.3 Ma CC pluton age represents the oldest Taconic arc-related plutonic activity yet documented in Western Newfoundland and provides a minimum age for the intruded CC ophiolite basement and initiation of westerly vergent subduction within the peri-Laurentian Iapetus Ocean. This confirms the Early Cambrian CC mafic–ultramafic basement is significantly older than the juxtaposed SSZ BOIC, which formed by later rifting of the CC forearc along younger forearc spreading center in the Late Cambrian by ca. 488.3 Ma. After subduction initiation a prolonged early period CC forearc silicic magmatism lasted at least ∼ 11.6 Ma until ca. 502.7 Ma, a range consistent with age spans of magmatism in modern juvenile forearcs. We also reinvestigated the Central Newfoundland Twillingate Granite batholith thought to be one of the earliest major felsic batholiths formed within the adjacent juvenile arc massif of the Notre Dame Subzone, part of the same peri-Laurentian arc. We determined a precise 3-sample composite age of 504.3 ± 1.8 Ma that signals the formation of earliest Notre Dame arc edifice developed by Middle Cambrian. It overlaps the end-stage CC forearc plagiogranite magmatism and places a minimum mid-Cambrian age constraint on intruded ophiolitic arc tholeiitic and boninitic pillow lavas of the Sleepy Cove and correlated Lushs Bight volcanics, suggesting basement continuity with the CC.