We have investigated crustal thickness and composition across the southeastern Caribbean plate boundary with the receiver function technique. We used teleseismic data recorded by a temporary broadband array deployed under the BOLIVAR project and the permanent national seismic network of Venezuela. We used the primary P-to-S conversion and crustal reverberations to estimate crustal thickness and average crustal VP/VS ratio over the region. We observe large variations in crustal thickness and Poisson's ratio. Estimated Moho depth ranges from ∼16 km beneath the southeastern Caribbean Sea to ∼52 km beneath northeastern Venezuela and the Venezuelan Andes. There is a good correlation between crustal structure and tectonic terranes. Data from the Precambrian Guayana Shield suggest that the underlying crustal structure is relatively uniform with a moderate thickness (∼37 km) and an intermediate composition. A thick crust is found below the foreland basins. The two mountain systems in northern Venezuela, the Serrania del Interior and the Serrania del Falcon, have a thin crust with are composition and are likely dynamically supported by elastic rebound or underthrusting of the oceanic plateau that characterizes the southem Caribbean. On the other hand, the Venezuelan Andes and Perija Range on the western side of the country are probably isostatically balanced by thick crustal roots.