Determining the crustal structure of ocean island volcanoes is important to understand the formation and tectonic evolution of the oceanic lithosphere and tectonic swells in marine settings, and to assess seismic hazard in the islands. The Azores Archipelago is located near a triple junction system and is possibly under the influence of a mantle plume, being at the locus of a wide range of geodynamic processes. However, its crustal structure is still poorly constrained and debated due to the limited seismic coverage of the region and the peculiar linear geometry of the islands. To address these limitations, in this study we invert teleseismic Rayleigh wave ellipticity measurements for 1-D shear wave speed (VS) crustal models of the Azores Archipelago. Moreover, we test the reliability of these new models by using them in independent moment tensor inversions of local seismic data and demonstrate that our models improve the waveform fit compared to previous models. We find that data from the westernmost seismic stations used in this study require a shallower Moho depth (∼10 km) than data from stations in the eastern part of the archipelago (∼13–16 km). This apparent increase in the Moho depth with increasing distance from the mid-Atlantic ridge (MAR) is expected. However, the rate at which Moho deepens away from the MAR is greater than that predicted from a half-space cooling model, suggesting that local tectonic perturbations have modified crustal structure. The 1-D VS models obtained beneath the westernmost seismic stations also show higher wave speeds than for the easternmost stations, which correlates well with the ages of the islands except Santa Maria Island. We interpret the relatively low VS profile found beneath Santa Maria Island as resulting from underplating, which agrees with previous geological studies of the island. Compared to a recent receiver function study of the region, the shallow structure (top ∼2 km) in our models shows lower shear wave speed, which may have important implications for future hazard studies of the region. More generally, the new seismic crustal models we present in this study will be useful to better understand the tectonics, seismicity, moment tensors and strong ground motions in the region.