Detrital zircons from pre-orogenic Upper Ordovician to Devonian low-grade metasedimentary rocks have been dated by laser ablation–inductively coupled plasma mass spectrometry (LA–ICP-MS) to: (1) constrain the variations of zircon age populations within the autochthonous sequences of NW Iberia; (2) compare U–Pb detrital zircon ages with previous data; (3) test the hypothesis of the Armorica microplate as a peri-Gondwanan terrane separated from Gondwana. The similarity in the ages of detrital zircons found in the Palaeozoic samples studied here to those published for the Upper Proterozoic, Lower Cambrian and Lower Ordovician sediments of NW Iberia argues against the separation of Armorica, and points to a common source area for all of the Palaeozoic detrital formations of NW Iberia, the West African craton and the surrounding Pan-African belts. LA–ICP-MS U–Pb dating of zircons from a synorogenic flysch preserved in klippen in the core of a syncline establishes a maximum depositional age for this deposit as Early Namurian. This age is also a maximum age limit for thrusting and refolding in this part of the Iberian Massif. Correlation of the zircon age populations with published ages confirms the link between the emplacement of the allochthonous complexes of NW Iberia and synorogenic sedimentation.