The proto-Andean margin of Argentina consists of several suspect terranes, the origins of which are disputed. The Cuyania (greater Precordillera) suspect terrane was originally interpreted to be of southeast Laurentian affinity, but more recently a southwestern Gondwanan provenance has been argued. Both potential source regions comprise Mesoproterozoic rocks, but we show they are isotopically distinct, using previously published zircon Lu-Hf data. Detrital zircon εHf data from southwestern Gondwana (Namaqua-Natal belt) show no correlation with new zircon U-Pb and Lu-Hf data from Cuyania, suggesting that Gondwana was not the source of these sediments. Rather, detrital zircons from Cambrian strata in Cuyania yield Mesoproterozoic zircons with depleted εHf that correlate to the Grenville margin of Laurentia, and a ca. 535 Ma zircon population sourced directly from rift-related rocks of the Ouachita Embayment, thus recording rifting and drifting of Cuyania from Laurentia. By contrast, zircons from Middle to Late Ordovician strata of Cuyania record a larger range of εHf values, correlated with Western Sierras Pampeanas Mesoproterozoic basement inliers of Argentina. These synorogenic clastic deposits record the Ordovician arrival of Cuyania at the proto-Andean margin of Gondwana. The new data require the terrane boundaries of Cuyania to be redefined, thereby excluding Western Sierras Pampeanas basement inliers. The results verify the Laurentian microcontinent model for the origin of Cuyania.