Flysch-type, syn-orogenic deposits of Carboniferous age occur in relation to the emplacement of a large allochthonous nappe stack in the Variscan belt of NW Iberia. New U–Pb age populations of detrital zircons obtained using laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS) are considered together with others from previously dated samples to establish the relationships between sedimentation and thrusting. The age populations of four syn-orogenic formations are compared with those of the pre-orogenic sequence in the Autochthon and Parautochthon, representing the Gondwanan passive margin, and in the Allochthon, formed by peri-Gondwanan and oceanic terranes. In addition, a new structural study has been carried out to understand the relationships between the syn-orogenic deposits and the development of Variscan structures. The aims are to identify the sources of sediments and to establish the relationship between Variscan structural evolution and syn-orogenic sedimentation. Development of a forebulge outwards from the allochthonous front, deduced from the structural study, suggests the existence of depocentres that hosted the syn-orogenic sediments. Together with the trend shown by the more recent zircons in each formation, that are younger towards the external zones, the data suggest that sedimentation occurred in progressively migrating depocentres formed in front of the allochthonous wedge during its emplacement. The zircon age populations point to the Allochthon as the main source of detritus for the syn-orogenic basins, with perhaps a limited participation of the Parautochthon and Autochthon in the younger formations.