Concentrations of polychlorinated biphenyls (PCBs) in the Delaware River currently exceed the Water Quality Criteria of 16 pg/L for the sum of PCBs due in part to atmospheric deposition. The purpose of this work was to use a source apportionment tool called Positive Matrix Factorization (PMF) to identify the sources of PCBs to the atmosphere in this area and determine whether their concentrations are declining over time. The data set was compiled by the Delaware Atmospheric Deposition Network (DADN) from samples taken in Camden, NJ from 1999 to 2011 and New Brunswick, NJ from 1997 to 2011. The PMF analysis revealed four resolved factors at each site. The factors that dominate the PCB burden in the atmosphere at both Camden and New Brunswick resemble Aroclor 1242. These factors declined in concentration during some portions of the monitoring period, but this decline slowed or stopped during 2003-2011. None of the factors displayed consistent declines in concentration throughout the monitoring periods, and some factors actually increased in concentration during some periods. This suggests natural attenuation alone will not control atmospheric PCB concentrations, and additional efforts are needed to control PCB atmospheric emissions as well as the numerous other sources of PCBs to the estuary.