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Three field campaigns were conducted before, during, and after the 2010 World Expo in Shanghai, aiming to understand the response of secondary aerosol components to both control measures and human activities. In spring, PM</sub>2.5</sub> (particulate matter) averaged 34.5 &plusmn; 20.9 μg m⁻³ with a severe pollution episode influenced by a floating dust originating from northwestern China on 26–28 April, right before the opening of the expo. With the approaching expo a significant increasing trend of SNA (SO₄^2&minus;, NO₃^&minus;, and NH₄⁺) concentrations was observed from 22 April to 2 May, attributed to the enhanced human activities. Nitrate had the most significant daily increasing rate of 1.1 μg m⁻³d⁻¹ due to enhanced vehicle emission. In summer, two intensive pollution episodes were found to be a mixed pollution of SNA with biomass burning due to loose control of post-harvest straw burning. In the autumn phase of the expo, before the closing of the expo (20–30 October), the air quality over Shanghai was much better than ever before. However, the air quality rapidly plummeted as soon as the expo was announced closed. SNA increased 3–6 fold to be 42.1 and 68.2 μg m⁻³ on 31 October and 1 November, respectively, as compared to 20–30 October. Of which, nitrate increased most ~5–8 fold, indicating the serious impact from enhanced vehicle emission. Compared to the spring and summer of 2009, NO₃^&minus; increased 12–15% while SO₄^2&minus; showed reductions of 15–30%. Continuous desulfurization of SO₂ emission from power plants in recent years was responsible for the lowered SO₄^2&minus;, while increased traffic emission from the tremendous number of expo visitors was the major contributor to the increased NO₃^&minus;. Compared to the autumn of 2009, all the ion components increased in 2010, owing to the lifting of emission control measures after the expo. SO₄^2&minus; was found least increased while NO₃^&minus; and Ca²⁺ had tremendous increases of 150 and 320%, respectively. The anthropogenic Ca as a tracer from construction dust increased from 2.88 &plusmn; 1.85 μg m⁻³ during the expo to 6.98 &plusmn; 3.19 μg m⁻³ during the post-expo period, attributed to the resumption of construction works after the expo. The lack of successive control measures with the loose regulations after the expo were responsible for this jump of the bad quality. The ratio of NO₃^&minus;/SO₄^2&minus; in PM_2.5 over Shanghai had a significant increasing trend from ~0.3 in the early 2000s to more than 1.0 in 2010, indicating the increasing role of mobile sources. Reducing NO_x emission will be China's priority in the future in order to improve the air quality over the megacities. In addition, lowering mineral aerosol components (e.g., Ca²⁺) was also demonstrated to be beneficial for alleviating air pollution in China. This study demonstrated that stringent emission control measures aiming at mega-events in China could achieve positive benefits on improving the air quality in a short term. However, persistent efforts of curbing the anthropogenic emission remain a long way to go in the future.