A well-known second-order mass extinction took place during the Pliensbachian and Toarcian Stages of the Early Jurassic. First recognized as a minor Pliensbachian peak in the global extinction rate, it has alternatively been interpreted as a regional response to the early Toarcian oceanic anoxic event. Detailed studies established it as a global long-term event spanning five successive ammonoid zones. Here we present a revised time scale based on high-precision U-Pb ages resolved to the zone level, which suggests that elevated extinction rates were sustained for about 4 m.y. and peak extinction occurred at 183 Ma. Recent isotopic dating of flood basalts from the southern Gondwanan Karoo and Ferrar provinces documents a culmination in volcanic activity ca. 183 Ma. The onset of volcanism is recorded as an inflection and start of a rapid rise of the seawater 87Sr/86Sr curve. The synchrony of voluminous flood basalt eruptions and biotic crises, as already noted for three of the major mass extinctions, permits a causal relationship, which in this case may be mediated by widespread oceanic anoxia.