The Potiguar Basin is a ∼6,000 m thick aborted NE-trending rift that was formed during the Cretaceous in the continental margin of northeastern Brazil. Its ∼E–W-trending offshore faults form part of the successful continental margin rift that evolved into the South Atlantic Ocean. The region represents one of the most significant pre-Pangea breakup piercing points between eastern South America and West Africa. We used gravity, aeromagnetic, and geological data to assess the role of reactivated Precambrian shear zones and major terrain boundaries in the development of the Potiguar Basin from the Cretaceous to the Cenozoic. We also looked for possible links between these structures in northeastern Brazil and their continuation in West Africa. Our results indicate that the major fault systems of the Potiguar Basin were superimposed on the Precambrian fabric. Both gravity and magnetic maps show lineaments related to the shear zones and major terrain boundaries in the Precambrian crystalline basement, which also characterize the architecture of the rift. For example, the Carnaubais fault, the master fault of the rift system, represents the reactivation of the Portalegre shear zone, the major tectonic boundary between Precambrian terrains in the crystalline basement. In addition, part of the Moho topography is controlled by these shear zones and developed during the period of main rift extension in the Neocomian. The shear zones bounding the Potiguar rift system continue in West Africa around and underneath the Benue Basin, where fault reactivation also took place.