The Ordovician-Silurian transition (OST) hosted profound and frequent changes in the atmospheric-terres trial-oceanic-climatic system (ATOCS). Previous studies have found contrasting stages for such changes, primarily based on hiatus-interrupted sections. However, the dominant driving factors and mechanisms reconciling such frequent changes remain controversial. Mercury isotopes, which undergo both massdependent and mass-independent fractionation, can provide critical insights into the deep-time ATOCSs, especially for those impacted by large igneous provinces (LIPs) events. Here, we build a highresolution multi-proxy record of Hg (concentrations and isotopic compositions) combined with organic carbon isotopes (d13Corg) and whole-rock geochemical data (including trace elements and phosphorus) from continuous cores in the Yangtze Platform, South China. Our data, combined with reported ones, indicate the occurrence of LIP eruptions against localized volcanism, and four successive, yet contrasting stages of ATOCSs during the OST. Moreover, we identified the coupling between two-pulse LIP magmatism and extreme ATOCSs, each with special pCO2, weathering rate, primary productivity, redox condition, climatic mode, and biotic evolution. For stage I, the first pulse of LIP magmatism triggered global warming, enhanced terrestrial weathering, oceanic acidification, eutrophication, anoxia, P recycling, and thereby widespread deposition of black shales. During stage II, the Hirnantian glaciation and oxygenation arose from the intense chemical weathering and black shale deposition of stage I; slashed terrestrial weathering and oceanic oxygenation facilitated CO2 accumulation. In stage III, another pulse of LIP magmatism triggered the de-glaciation, and the ATOCS was largely similar to that of stage I. This led to another round of oxygenation and positive d13Corg excursion in stage IV. Compared with the environmental pressure by the peculiar ATOCS of each stage, their transitions might have been more devastating in triggering the prolonged Late Ordovician Mass Extinction (LOME). Moreover, limited biotic recovery was possible in the later portion of stages I and III. The multi-proxy study of continuous strata of the OST provides an excellent framework for better illuminating LIPs' essential role in driving the "roller-coaster" behavior of the ATOCS and thus biotic crisis during the pivotal period of the OST. (c) 2023 China University of Geosciences (Beijing) and Peking University. Production and hosting by Elsevier B.V. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/ licenses/by-nc-nd/4.0/).