We present the results of the analysis of new wide-angle seismic data across the Caribbean-South American plate boundary in eastern Venezuela at about 65W. The ∼500 km long profile crosses the boundary in one of the few regions dominated by extensional structures, as most of the southeastern Caribbean margin is characterized by the presence of fold and thrust belts. A combination of first-arrival traveltime inversion and simultaneous inversion of PmP and Pn arrivals was used to develop a P wave velocity model of the crust and the uppermost mantle. At the main strike-slip fault system, we image the Cariaco Trough, a major pull-apart basin along the plate boundary. The crust under the Southern Caribbean Deformed Belt exhibits a thickness of ∼15 km, suggesting that the Caribbean Large Igneous Province extends to this part of the Caribbean plate. The velocity structures of basement highs and offshore sedimentary basins imaged by the profile are comparable to those of features found in other parts of the margin, suggesting similarities in their tectonic history. We do not image an abrupt change in Moho depth or velocity structure across the main strike-slip system, as has been observed elsewhere along the margin. It is possible that a terrane of Caribbean island arc origin was accreted to South America at this site and was subsequently bisected by the strike-slip fault system. The crust under the continental portion of the profile is thinner than observed elsewhere along the margin, possibly as a result of thinning during Jurassic rifting.