A total of 120 air samples were collected at three urban and one rural location in Beijing, China in the summers of 2007−2010, and before, during, and after the Beijing 2008 Olympic Games (BOG), in order to assess the effectiveness of long-term and short-term emission-control measures in reducing polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) in the atmosphere. During the BOG (August, 2008), the PCDD/Fs concentrations decreased to an average value of 1150 fg m−3 (63 fg I-TEQ m−3), which was reduced by approximately 70% from the average in 2007 and by 29% from that in July 2008, before the Olympic event began. Although 2009−2010 levels of PCDD/Fs were significantly higher than 2008, the overall temporal trend was decreasing for summer months during the sampling campaign period. The apparent half-lives of atmospheric PCDD/Fs were estimated to be 3.2−5.8 years by statistically regressing the logarithm PCDD/Fs concentrations versus the number of years passed since 2006. The air concentrations of total suspended particulates (TSP) during the BOG ranged between 135 and 183 μg m−3, showing a 52% reduction from 2007 and 26% decrease from those prior to the Olympic event. No significant relationships were found between meteorological parameters (temperature, humidity, and wind speed) and PCDD/Fs or TSP during the BOG, whereas the PCDD/Fs concentrations were significantly dependent on the air quality (p < 0.05, positive against TSP and negative against visibility). This work is one of few temporal trend studies of atmospheric PCDD/Fs in mainland China, and provides unique insight into the effects of large-scale control measures in improving air quality and reducing one of the most ubiquitous and toxic organic pollutants in the environment.