The church of Santa María del Naranco is an important monument from the pre-Romanesque period of Asturian art. Here we present research that locates the probable source of travertine used in the construction of a vault within this monument. Since the genesis of this travertine is associated with spring activity, and archival evidence suggests that stone procurement during this period tended to be local, we surveyed existing carbonated aquifers within a 5-km radius of the monument. We identified a spring (Sopeña) with an associated outcrop of discontinuous travertine that appeared to have been quarried in the past. We conducted X-ray powder diffraction, electron microprobe, and inductively coupled plasma mass spectrometry analyses of samples extracted from the suspected travertine source, an additional more distant travertine quarry for comparison, and the vault. Matching mineralogy and geochemistry indicate that the Sopeña travertine was the probable source of rock material used in the construction of the vault. This study provides insight into local ancient monument construction and can assist in procuring original stone material for historical restoration.