We report Sr, Nd and Pb isotopic compositions of mid-Proterozoic anorthosites and related rocks (1.45-1.65 Ga) and of younger olivine diabase dikes (1.4 Ga) from two complexes on either side of the Grenville Front in Labrador. Anorthositic or diabasic samples from the Mealy Mountains (Grenville Province) and Harp Lake (Nain-Churchill Provinces) complexes have very similar major, minor and trace element compositions, but distinctly different isotopic signatures. All Mealy Mountains samples have I_Sr = 0.7025−0.7033, ε_Nd = +0.6 to +5.6 and Pb isotopic compositions consistent with derivation from a mantle source depleted with respect to Nd/Sm and Rb/Sr. Pb isotopic compositions for the Mealy Mountains samples are slightly more radiogenic than model mantle compositions. All Harp Lake samples have I_Sr = 0.7032−0.7066, ε_Nd = −0.3 to −4.4 and variable, but generally unradiogenic ²⁰⁷Pb/²⁰⁴Pb and ²⁰⁶Pb/²⁰⁴Pb compared to model mantle, suggesting mixing between a mantle-derived component and a U-depleted crustal contaminant. Crustal contaminants are probably a variety of Archean high-grade quartzofeldspathic gneisses with low U/Pb ratios and include a component that must be isotopically similar to the early Archean (>3.6 Ga) Uivak gneisses of Labrador or the Amitsoq gneisses of west Greenland. This would imply that the ancient gneiss complex of coastal Labrador and Greenland is larger than indicated by present surface exposure and may extend in the subsurface as far west as the Labrador Trough. If Harp Lake and Mealy Mountains samples were subjected to the same degree of contamination, as suggested by their chemical similarities, then the Mealy contaminants must be much younger, probably early or middle Proterozoic in age. The Labrador segment of the Grenville Front, therefore, appears to coincide with the southern margin of the Archean North Atlantic craton and may represent a pre mid-Proterozoic suture.