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Although many sources of atmospheric CO2 have been identified, the major sinks are best understood in a deep-time context. Here, we focus on two Large Igneous Provinces (LIPs), the Central Atlantic Magmatic Province (CAMP) situated in the low latitude humid zone ~201.6 Ma and the Karoo-Ferrar located at high southern latitudes ~183 Ma. We use soil carbonate, lithologic, δD of n-alkanes, Sr data, and modeling to examine how these eruptions, hydrological cycling, and weathering impacted global atmospheric CO2, carbon cycling, and biotic extinction at the ETE and T-OAE hyperthermals. CAMP largely erupted in the tropics, doubled atmospheric CO2 from ~2,500 – 5,000 ppm at the ETE (observed in soil carbonates with an onset <1000 and a duration of <~20 ky) and rapidly sequestered CO2 (< 2,500 ppm) as recorded in Newark Supergroup basins (eastern US). These same strata preserve variations in the lake level expression of the climatic precession cycle based on lithology and δD. High cyclicity variance tracked high pCO2 (>~4000 ppm) and drove insolation-paced increases in precipitation. Leaf wax δD shows significant variability, reflecting an enhanced hydrological cycle at the ETE with repeated sudden shifts in relative evaporation for ~1 Myr. In marine strata, 87Sr/86Sr and 187Os/188Os values track changes in pCO2, suggesting a terrestrial/marine linkage through continental weathering, CO2, and runoff. Despite the northward movement of these basins into the arid belt, our data suggest lower evaporation relative to precipitation driven by lower temperatures, consistent with lower pCO2 due to CAMP weathering, which modeling estimates to have increased 6 to 10-fold for >1.6 Myr after the eruptive phase. Release of CO2 from the Karoo-Ferrar LIP similarly enhanced the hydrological cycle as evidenced from sedimentary observations (e.g., fine-scale turbidites and debris flow deposits) in Yorkshire (UK). The onset of the carbon isotope excursion at the T-OAE lasts 0.5 Myr with a 1.5 Myr duration modulated by astronomical pacing. Our leaf wax δD from the same strata show a transient enhancement in the hydrological cycle. Although the Karoo-Ferrar has a limited drawdown potential when compared with CAMP‐type basalts because of its higher latitude location, Toarcian weathering rates may have increased 2 to 5-fold, acting as a net sink 1–2 Myr after eruptions ceased.