The lithospheric architecture of the Pyrenees is still uncertain and highly debated. Here, we provide new constraints from a high-resolution 3-D S-wave velocity model of the Pyrenees and the adjacent foreland basins. This model is obtained from ambient noise tomography on records of temporary and permanent seismic arrays installed in southwestern France and northern Spain. We first computed group velocity maps for Rayleigh waves in the 5 to 55 s period range using noise correlation stacks at 1500-8500 station pairs. As the crust is very heterogeneous, poor results were obtained using a single starting model in a linearized inversion of group velocity dispersion curves for the shear wave structure. We therefore built a starting model for each grid node by full exploration of the model space. The resulting 3-D shear wave velocity model is compared to data from previous geophysical studies as a validation test. Despite the poor sensitivity of surface waves to seismic discontinuities, the geometry of the top of the basement and the Moho depth are retrieved well, except along the Cantabrian coast. Major reflectors of the ECORS deep seismic sounding profiles in the central and western Pyrenees coincide with sharp velocity gradients in our velocity model. We retrieve the difference between the thicker Iberian crust and the thinner European crust, the presence of low-velocity material of the Iberian crust underthrust beneath the European crust in the central Pyrenees, and the structural dissymmetry between the South Pyrenean Zone and the North Pyrenean Zone at the shallow crustal level. In the Labourd-Mauléon-Arzacq region (western Pyrenees), there is a high S-wave velocity anomaly at 20-30 km in depth, which might explain the positive Bouguer anomaly of the Labourd Massif. This high-velocity lower crust, which is also detected beneath the Parentis area, might be an imprint of the Albian-Aptian rifting phase. The southeastern part of the Massif Central has an unusual velocity structure, with a very shallow Moho (21-25 km) above an uppermost mantle with anomalously low shear wave velocity.