The geodynamic evolution of the South Armenian Block (SAB) within the Tethyan realm during the Palaeozoic to present-day is poorly constrained. Much of the SAB is covered by Cenozoic sediments so that the relationships between the SAB and the neighbouring terranes of Central Iran, the Pontides and Taurides are unclear. Here we present new geochronological, palaeomagnetic, and geochemical constraints to shed light on the Gondwanan and Cimmerian provenance of the SAB, timing of its rifting, and geodynamic evolution since the Permian. We report new 40Ar/39Ar and zircon U-Pb ages and compositional data on magmatic sills and dykes in the Late Devonian sedimentary cover, as well as metamorphic rocks that constitute part of the SAB basement. Zircon age distributions, ranging from ∼3.6 Ga to 100 Ma, firmly establish a Gondwanan origin for the SAB. Trondhjemite intrusions into the basement at ∼263 Ma are consistent with a SW-dipping active continental margin. Mafic intraplate intrusions at ∼246 Ma (OIB) and ∼234 Ma (P-MORB) in the sedimentary cover likely represent the incipient stages of breakup of the NE Gondwanan margin and opening of the Neotethys. Andesitic dykes at ∼117 Ma testify to the melting of subduction-modified lithosphere. In contrast to current interpretations, we show that the SAB should be considered separate from the Taurides, and that the Armenian ophiolite complexes formed chiefly in the Eurasian forearc. Based on the new constraints, we provide a geodynamic reconstruction of the SAB since the Permian, in which it started rifting from Gondwana alongside the Pontides, likely reached the Iranian margin in Early Jurassic times, and was subject to episodes of intraplate (∼189 Ma) and NE-dipping subduction-related (∼117 Ma) magmatism