Detrital zircon grains from Cambrian–Lower Ordovician sandstones and quartzites sampled in the Pyrenees were dated by LA-ICPMS in order to assess their provenance sources. Resulting age distributions are compared to other available datasets from neighbouring margins, such as Morocco, the Iberian Peninsula, southern France and Sardinia. Kolmogorov-Smirnov (K-S) test and Crystallization Age-Depositional Age (CA-DA) diagrams were used to compare zircon populations estimating their possible correlation with the arc/rift/drift geodynamic evolution of the northwestern Gondwana margin. During Terreneuvian times, zircon populations allowed the distinction of i) a southwesternmost edge (Atlas-Ossa-Morena Rift) mostly influenced by Panafrican and Anti-Atlasian sources (ca. 0.63–0.54), ii) a northeasternmost edge (Sardinia) recording the influence of the Saharan Metacraton and the Arabian Nubian Shield, with an distinct Stenian–Tonian shift (ca. 1.25–0.85Ga) and iii) an intermediate palaeogeographic transect, where lies the Central Iberian, West Asturian-Leonese and Cantabrian Zones, the Montagne Noire and the Pyrenees sharing similar populations and a chronologically progressive influence from Anti-Atlasian/Panafrican to Saharan Metacraton/Arabian Nubian Shield sources. This gradual modification in zircon percentage populations supports similar trends based on climatically sensitive indicators, biogeographic patterns of Cambrian Epoch 2 archaeocyathan and microfossil assemblages, and laterally correlatable episodes of carbonate production, all of them pointing to a Cambrian setting for the Pyrenean Basin between the Montagne Noire (Occitan Domain) and the Sardinian margins of NW Gondwana. The Terreneuvian zircon patterns recorded in the Pyrenees gradually evolved from Cambrian Epoch 2 to Early Ordovician times, reflecting the geodynamic evolution from Panafrican and Cadomian arc-related to rift-dominant conditions. During Furongian and Ordovician times, the relative percentage of zircon populations led to a more spread age curve, characteristic of extensional settings and pointing to rift (passive margin) conditions