A geochronology and Hf isotope study, using laser ablation-ICP-MS analysis of zircon grains, has been conducted to date felsic volcanic rocks from the Portuguese sector of the Iberian Pyrite Belt and to establish possible sources for these rocks. The ages obtained range from the Famennian to the Tournaisian, with the oldest ages reported in the Belt so far being identified in its southwestern part (Cercal area). Results also indicate that within each area, volcanism may have extended for significant periods of time. This suggests that caution is needed in interpreting possible migration trends for the volcanism, as the exact stratigraphic position of the sampled rocks is not always clear. Despite of this, the new data, coupled with previously reported information, suggests that volcanism migrated within the basin from the southwest to the northeast (present day coordinates). Projection from initial zircon εHf values towards the depleted mantle evolution curve, via an intermediate reservoir, allows the calculation of Hf protolith model ages that are predominantly Meso-Proterozoic. This is compatible with acid magmas resulting from the fusion of Phyllite-Quartzite (PQ) Formation metasedimentary rocks, which are beneath the volcanic rocks. This is because zircon grains from one PQ Formation sample provided Late Neo-Proterozoic ages and Paleo-Proterozoic to Late Archean U-Pb ages, and the Hf isotope signatures of these zircons can be expected to mix during fusion and result in protolith model ages that would be intermediate between the two U-Pb age populations, as recorded. Further supporting this source for the magmas, the distribution of U-Pb ages of (pre-Variscan) inherited zircon grains in the volcanic rocks is very similar to that shown by the detrital zircon grains from a PQ sample.