By compiling wide-angle seismic velocity profiles along the ∼400-km-long Lofoten–Vesterålen continental margin off Norway, and integrating them with an extensive seismic reflection data set and crustal-scale two-dimensional gravity modelling, we outline the crustal margin structure. The structure is illustrated by across-margin regional transects and by contour maps of depth to Moho, thickness of the crystalline crust, and thickness of the 7+ km/s lower crustal body. The data reveal a normal thickness oceanic crust seaward of anomaly 23 and an increase in thickness towards the continent–ocean boundary associated with breakup magmatism. The southern boundary of the Lofoten–Vesterålen margin, the Bivrost Fracture Zone and its landward prolongation, appears as a major across-margin magmatic and structural crustal feature that governed the evolution of the margin. In particular, a steeply dipping and relatively narrow, 10–40-km-wide, Moho-gradient zone exists within a continent–ocean transition, which decreases in width northward along the Lofoten–Vesterålen margin. To the south, the zone continues along the Vøring margin, however it is offset 70–80 km to the northwest along the Bivrost Fracture Zone/Lineament. Here, the Moho-gradient zone corresponds to a distinct, ∼25-km-wide, zone of rapid landward increase in crustal thickness that defines the transition between the Lofoten platform and the Vøring Basin. The continental crust on the Lofoten–Vesterålen margin reaches a thickness of ∼26 km and appears to have experienced only moderate extension, contrasting with the greatly extended crust in the Vøring Basin farther south. There are also distinct differences between the Lofoten and Vesterålen margin segments as revealed by changes in structural style and crustal thickness as well as in the extent of elongate potential-field anomalies. These changes may be related to transfer zones. Gravity modelling shows that the prominent belt of shelf-edge gravity anomalies results from a shallow basement structural relief, while the elongate Lofoten Islands belt requires increased lower crustal densities along the entire area of crustal thinning beneath the islands. Furthermore, gravity modelling offers a robust diagnostic tool for the existence of the lower crustal body. From modelling results and previous studies on- and off-shore mid-Norway, we postulate that the development of a core complex in the middle to lower crust in the Lofoten Islands region, which has been exhumed along detachments during large-scale extension, brought high-grade, lower crustal rocks, possibly including accreted decompressional melts, to shallower levels.