The New Albany-Chesterian petroleum system of the Illinois basin is a well-constrained system from which petroleum charges and losses were quantified through a material-balance assessment. This petroleum system has nearly 90,000 wells penetrating the Chesterian section, a single New Albany Shale source rock accounting for more than 99% of the produced oil, well-established stratigraphic and structural frameworks, and accessible source rock samples at various maturity levels. A hydrogen index (HI) map based on Rock-Eval analyses of source rock samples of New Albany Shale defines the pod of active source rock and extent of oil generation. Based on a buoyancy-drive model, the system was divided into seven secondary-migration catchments. Each catchment contains a part of the active pod of source rock from which it derives a petroleum charge, and this charge is confined to carrier beds and reservoirs within these catchments as accountable petroleum, petroleum losses, or undiscovered petroleum. A well-constrained catchment with no apparent erosional or leakage losses is used to determine an actual petroleum charge from accountable petroleum and residual migration losses. This actual petroleum charge is used to calibrate the other catchments in which erosional petroleum losses have occurred. Petroleum charges determined by laboratory pyrolysis are exaggerated relative to the actual petroleum charge. Rock-Eval charges are exaggerated by a factor of 4-14, and hydrous-pyrolysis charges are exaggerated by a factor of 1.7. The actual petroleum charge provides a more meaningful material balance and more realistic estimates of petroleum losses and remaining undiscovered petroleum. The total petroleum charge determined for the New Albany-Chesterian system is 78 billion bbl, of which 11.4 billion bbl occur as accountable in place petroleum, 9 billion bbl occur as residual migration losses, and 57.6 billion bbl occur as erosional losses. Of the erosional losses, 40 billion bbl were lost from two catchments that have highly faulted and extensively eroded sections. Anomalies in the relationship between erosional losses and degree of erosion suggest there is potential for undiscovered petroleum in one of the catchments. These results demonstrate that a material-balance assessment of migration catchments provides a useful means to evaluate and rank areas within a petroleum system. The article provides methodologies for obtaining more realistic petroleum charges and losses that can be applied to less data-rich petroleum systems.