The Paleocene-Eocene Thermal Maximum (PETM) (̃56 Ma) was a ̃170,000-y (̃170-kyr) period of global warming associated with rapid and massive injections of 13C-depleted carbon into the ocean-atmosphere system, reflected in sedimentary components as a negative carbon isotope excursion (CIE). Carbon cycle modeling has indicated that the shape and magnitude of this CIE are generally explained by a large and rapid initial pulse, followed by ̃50 kyr of 13C-depleted carbon injection. Suggested sources include submarine methane hydrates, terrigenous organic matter, and thermogenic methane and CO2 from hydrothermal vent complexes. Here, we test for the contribution of carbon release associated with volcanic intrusions in the North Atlantic Igneous Province. We use dinoflagellate cyst and stable carbon isotope stratigraphy to date the active phase of a hydrothermal vent system and find it to postdate massive carbon release at the onset of the PETM. Crucially, however, it correlates to the period within the PETM of longer-term 13C-depleted carbon release. This finding represents actual proof of PETM carbon release from a particular reservoir. Based on carbon cycle box model [i.e., Long-Term Ocean-Atmosphere-Sediment Carbon Cycle Reservoir (LOSCAR) model] experiments, we show that 4-12 pulses of carbon input from vent systems over 60 kyr with a total mass of 1,500 Pg of C, consistent with the vent literature, match the shape of the CIE and pattern of deep ocean carbonate dissolution as recorded in sediment records. We therefore conclude that CH4 from the Norwegian Sea vent complexes was likely the main source of carbon during the PETM, following its dramatic onset.