During recent decades concentrations of persistent organic pollutants (POPs) in the atmosphere have been monitored at multiple stations worldwide. We used three statistical methods to analyse a total of 748 time series of selected POPs in the atmosphere to determine if there are statistically significant reductions in levels of POPs that have had control actions enacted to restrict or eliminate manufacture, use and emissions. Significant decreasing trends were identified in 560 (75%) of the 748 time series collected from the Arctic, North America and Europe, indicating that the atmospheric concentrations of these POPs are generally decreasing, consistent with overall effectiveness of emission control actions. Statistically significant trends in synthetic time series could be reliably identified with the improved Mann-Kendall (iMK) test and the digital filtration (DF) technique in time series longer than 5 years. The temporal trends of new (or emerging) POPs in the atmosphere are often unclear because time series are too short. A statistical detrending method based on the iMK test was not able to identify abrupt changes in the rates of decline of atmospheric POP concentrations encoded into synthetic time series.