The link between mantle plumes and continental breakup remain a topic of debate. Here, a new 40Ar/39Ar age of 135.9 ± 1.2 Ma (2σ) and previous ages from the Bunbury Basalt – lava flows that are part of the Greater Kerguelen large igneous province (LIP) – reveal that >80% of magmatism in the southern Perth Basin was concomitant with the continental breakup of eastern Gondwana at ca. 137–136 Ma. New and existing isotope geochemical data show that only lithospheric and depleted asthenospheric sources were melted to form the Bunbury Basalt and most other early, ca. 147–124 Ma magmatic products part of the Greater Kerguelen LIP. All lines of evidence strongly point towards passive continental breakup of eastern Gondwana, including the restriction of 147–124 Ma magmatism to continental rifts, the lack of excess oceanic magmatism in this period and the >1000 km distance between the Kerguelen plume underneath Greater Indian lithosphere and the breakup nexus. It is not possible to reconcile the influence of a thermochemical plume with the observed geochemical, spatial and geochronological information. Instead, we posit that eastern Gondwana breakup occurred because it was proximal to the former suture zone associated with the ca. 550–500 Ma Kuunga Orogeny between Indo–Australia and Australo–Antarctica. Enrichment of the mantle with volatiles associated with subduction during the Kuunga Orogeny permitted partial melting when the continental crust was sufficiently attenuated in the Early Cretaceous. Repeated and protracted rifting of Greater India from Australo–Antarctic since the mid- Paleozoic eventually led to the rupture of the continental lithosphere and to mafic magmatism at ca. 137–136 Ma, approximately along the position of the former suture zone, without the influence of a mantle plume.