The effects of a large igneous province on the concentration of atmospheric carbon dioxide (PCO2) are mostly unknown. In this study, we estimate PCO2 from stable isotopic values of pedogenic carbonates interbedded with volcanics of the Central Atlantic Magmatic Province (CAMP) in the Newark Basin, eastern North America. We find pre-CAMP PCO2 values of ~2000 parts per million (ppm), increasing to ~4400 ppm immediately after the first volcanic unit, followed by a steady decrease toward pre-eruptive levels over the subsequent 300 thousand years, a pattern that is repeated after the second and third flow units. We interpret each PCO2 increase as a direct response to magmatic activity (primary outgassing or contact metamorphism). The systematic decreases in PCO2 after each magmatic episode probably reflect consumption of atmospheric CO2 by weathering of silicates, stimulated by fresh CAMP volcanics.