Recent studies have indicated that Eastern China might be a potential source region of increased atmospheric chlorofluorocarbons (CFCs). To investigate this possibility, a field measurement was carried out from October to December 2017 for identifying the ambient concentration levels of representative trichlorofluoromethane (CFC-11), dichlorodifluoromethane (CFC-12), trifluorotrichloroethane (CFC-113), and tetrafluorodichloroethane (CFC-114) at the residential and municipal solid waste (MSW) landfills and industrial sites in Eastern China. The ambient mixing ratios of CFCs at residential sites were almost within 20% enhancement of the global background sites. The highest levels of CFCs were observed at the MSW landfill sites. Moreover, CFC-11 and CFC-113 concentrations at MSW landfills, which were in service, were two times higher than that at completed MSW landfills. Mean concentrations of 322 pptv for CFC-11, 791 pptv for CFC-12, 91 pptv for CFC-113, and 16 pptv for CFC-114 at various industrial sites were higher than that at residential sites, but they were obviously lower than that at MSW landfills in use. A poor intercorrelation between the CFCs indicated that they did not come from the same sources. Higher concentrations measured in this study compared with background sites indicates that MSW landfills could be an unintentional emission source and there are still substantial amounts of CFCs being stored in banks that may discharge CFCs into the atmosphere in Eastern China.