A regional long-offset 2D seismic reflection program undertaken along the Labrador margin of the Labrador Sea, Canada, and complemented by the acquisition of coincident gravity data, has provided an extensive data set with which to image and model the sparsely investigated outer shelf, slope, and deepwater regions. Previous interpretation of the seismic data revealed the extent of Mesozoic and Cenozoic basins and resulted in the remapping of the basin configuration for the entire margin. To map the synrift package and improve understanding of the geometry and extent of these basins, we have undertaken joint seismic interpretation and gravity forward modeling to reduce uncertainty in the identification of the prerift basement, which varies between Paleozoic shelfal deposits and Precambrian crystalline rocks, with similar density characteristics. With this iterative approach, we have obtained new depth to basement constraints and have deduced further constraints on crustal thickness variations along the Labrador margin. At the crustal scale, extreme localized crustal thinning has been revealed along the southern and central portions of the Labrador margin, whereas a broad, margin-parallel zone of thicker crust has been detected outboard of the continental shelf along the northern Labrador margin. Our final gravity models suggest that Late Cretaceous rift packages from further south extend along the entire Labrador margin and open the possibility of a Late Cretaceous source rock fairway extending into the Labrador basins.