The atmosphere as a source of volatile organic compounds (VOCs) in shallow groundwater was evaluated over an area in southern New Jersey. Chloroform, methyl tertbutyl ether (MTBE), 1,1,1‐trichloroethane, tetrachloroethylene (PCE), and carbon disulfide (not a VOC) were detected frequently at low‐level concentrations in a network of 78 shallow wells in the surficial Kirkwood‐Cohansey aquifer system. The atmosphere was sampled for these compounds and only MTBE concentrations were high enough to potentially explain frequent detection in shallow groundwater. A mathematical model of reactive transport through the unsaturated zone is presented to explain how variations in unsaturated properties across the study area could explain differences in MTBE concentrations in shallow groundwater given the atmosphere as the source. Even when concentrations of VOCs in groundwater are low compared to regulatory concentration limits, it is critical to know the source. If the VOCs originate from a point source((), concentrations in groundwater could potentially increase over time to levels of concern as groundwater plumes evolve, whereas if the atmosphere is the source, then groundwater concentrations would be expected to remain at low‐level concentrations not exceeding those in equilibrium with atmospheric concentrations. This is the first analysis of VOC occurrence in shallow groundwater involving colocated atmosphere data.