The upper‐crustal anisotropy of the Cantabrian Mountains (North Spain) has been investigated using two independent but complementary methodologies: (a) shear‐wave splitting and (b) ambient seismic noise interferometry. For this purpose, we have processed and compared seismic data from two networks with different scales and recording periods. The shear‐wave splitting results show delay times between 0.06 and 0.23 s and spatially variable fast‐polarization directions. We calculate that the anisotropic layer has a maximum effective thickness of around 7.5 km and an average anisotropy magnitude of between 4% and 8%. Consistently, our ambient noise observations point to an anisotropy magnitude between 4% and 9% in the first 10 km of the crust. Our results show a clear correlation between the fast directions from both methods and the orientations of the local faults, suggesting that the anisotropy is mainly controlled by the structures. Furthermore, in the west of the study area, fast‐polarization directions tend to align parallel to the Variscan fabric in the crust, whereas to the east, in which the Alpine imprint is stronger, many fast directions are aligned parallel to east–west‐oriented Alpine features.