The North Natal valley (NNV), South Mozambique margin, is a key area for the understanding of the SW Indian Ocean history since the Gondwana break-up as its crustal nature and geometry strongly impacted the reconstruction of the paleogeography before the rifting. It is also of considerable importance for the understanding of the evolution of a margin system as the NNV is situated at the transition between divergent and strike-slip segments and at the conjunction of Oxfordian-Kimmeridgian Indian Ocean and the Valanginian-Aptian Atlantic one. As one part of the PAMELA project (PAssive Margins Exploration Laboratories), the NNV and the East Limpopo margin have been investigated during the MOZ3/5 cruise (2016), through the acquisition of 7 intersecting wide-angle profiles and coincident marine multichannel (720 traces) seismic as well as potential field data. Simultaneously, land seismometers were deployed in the Mozambique coastal plain (MCP), extending six of those profiles on land for about 100 km in order to provide information on the onshore-offshore transition. Wide-angle seismic data are of major importance as they can highlight constraints on the crustal structure of the margin and the position of the continent-ocean boundary in an area where the crustal nature is poorly known and largely controversial. The MOZ3/5 data set therefore reveals new essential constraints for kinematic reconstructions. This work presents results on the crustal structure from P-waves velocity modeling along two E-W wide-angle profiles (MZ1 and MZ2) through the NNV, from the Lebombo Monocline to the Mozambique Basin (MB), and crossing the Mozambique Fracture Zone (MFZ).The new geophysical data reveals an upper sedimentary sequence characterized by low velocities generally not exceeding 3 km/s, and up to 3 km thick where a major contouritic structure was observed. This feature formes together with several other contouritic structures, a N-S alignment just west of the MFZ, which produces high positive gravity anomalies, previously thought to be related to the magmatism that built the Galathea and Dana Plateaus. High velocity lenses are locally identified through the sedimentary layers and interpreted as inter-bedded volcanic sills. Furthermore, from the NNV to the MFZ, the underlying sequence is formed of a 3.0–3.5 km thick volcano-sedimentary sequence presenting important lateral changes in its seismic signature and characterized by a large velocity range (4.4 to 5.8 km/s), which partly reflects variations in the volcanic/sedimentary ratio laterally and with depth. At depth, an initially smoother and reduced eastward thinning of the crust occurs to the West below the continental shelf, from 34 to 31 km thick. The crustal thickness remains relatively constant of about 28–29 km along the Central Domain (CD), whereas a second and major region of thinning (26 to 12 km thick) is imaged West of the MFZ, in the southward prolongation of the Limpopo Corridor (LC). By contrast, as the eastern extremity, the crust is <10 km thick when reaching the MB. Crustal velocities reveal low velocity gradients, with atypical high velocities, increasing to 7.3 to 7.6 km/s at the base of the crust, and globally in the whole crust in the LC, just West of the MFZ. We interpreted the velocity architecture combined with the evidence of volcanism at shallower depths as indicative of an intensively intruded continental crust in the NNV, and discuss the particular segmentation of the longest profile (MZ1) in the kinematic context of both divergent and strike-slipe segments offshore Mozambique.Combining wide-angle and reflection seismic observations along these two profiles and the other MOZ3/5 lines, the data shows a coherent segmentation of the E-W crustal architecture off South Mozambique. These results along MZ1 and MZ2 profiles, combined with the previously published profiles, gives a 3D-view of the NNV, which becomes one of the most passive margins covered in the world by deep wide-angle seismic data.