The Triassic-Jurassic (T-J) boundary ca. 200 Ma represents one of the major mass extinction events of the Phanerozoic; however, the cause of this event remains controversial because of a paucity of geological evidence. In this study we present an isotopic record of osmium extracted from a bedded chert succession across the T-J boundary in the Kurusu section of Japan, deposited within a Paleo-Pacific (Panthalassa) deep basin. The data show a gradual decrease in seawater 187Os/188Os values during the Rhaetian, followed by a sharp increase in the latest Rhaetian, and a subsequent stable phase across the T-J boundary. The decreasing trend of 187Os/188Os values during the Rhaetian indicates a gradual increase in the relative supply rate of unradiogenic Os from the mantle associated with emplacement of the Central Atlantic Magmatic Province. The subsequent shift toward radiogenic values reflects an increased supply of radiogenic Os due to enhanced continental weathering. This interval marks more negative isotopic values of organic carbon, the onset of radiolarian faunal turnover, and conodont extinctions, indicating that the rapid increase in continental weathering rate was closely linked to the perturbation of the carbon cycle and the T-J biotic crisis.