Abstract We conducted 39 Ar diffusion experiments using potassium feldspar from the South Cyclades Shear Zone on Ios, in the Cyclades, Aegean Sea, Greece. Irradiated samples were step-heated in an ultra-high-vacuum resistance furnace attached to a mass spectrometer, thus also allowing 40 Ar/ 39 Ar geochronology. Conjoint inversion of these datasets allowed estimation of the relevant diffusion parameters, which were then used to forward model the effect of arbitrary temperature–time histories. Simulations used Monte Carlo methods to improve approximations to the observed age spectra. Two periods of rapid cooling could be inferred. The South Cyclades Shear Zone commenced operation during or shortly after the Eocene–Oligocene transition. Episodes of south-directed movement continued into Early Miocene time, however, with the footwall still hot enough to cause biotite ± garnet metamorphic mineral growth at the base of the overlying, already substantially exhumed, eclogite–blueschist unit. Since its footwall continued to cool, the South Cyclades Shear Zone was an extensional shear zone during both episodes of its operation.