Particulate air pollution is becoming a serious public health concern in urban cities of China. Association of disability-adjusted life years (DALYs) and economic loss with air pollution-related health effects demand quantitative analysis for correctional measures in air quality. This study applies an epidemiology-based exposure–response function to obtain the quantitative estimate of health impact of particulate matter PM2.5 and PM10 across 190 cities of China during years 2014–2015. The annual average concentration of PM2.5 and PM10 is 57 ± 18 μg/m3 (ranging from 18 to 119 μg/m3) and 97.7 ± 34.2 μg/m3 (ranging from 33.5 to 252.8 μg/m3), respectively. Based on the present study, the total estimated annual premature mortality due to PM2.5 is 722,370 [95% confidence interval (CI) = 322,716–987,519], 79% of which accounts for adult cerebrovascular disease (stroke) and ischemic heart disease (IHD). The premature mortality in megacities is very high, such as Chongqing (25,162/year), Beijing (19,702/year), Shanghai (19,617/year), Tianjin (13,726/year), and Chengdu (12,356/year). PM10 pollution has caused 1,491,774 (95% CI = 972,770–1,960,303) premature deaths (age >30) in China. Further, 3,614,064 cases of chronic bronchitis (CB); 13,759,894 cases of asthma attack among all ages; 191,709 COPD-related hospital admission (HA) cases; 499,048 respiratory-related HA; 357,816 cerebrovascular HA; and 308,129 cardiovascular-related HA due to PM10 pollution have been estimated during 2014–2015. Chongqing, Beijing, Baoding, Tianjin, and Shijiazhuang are the top five contributors to pollution-related mortality, accounting for 3.10, 2.71, 2.49, 2.20, and 2.02%, respectively, of the total deaths caused by PM10 pollution. The total DALYs associated with PM2.5 and PM10 pollution in China is 7.2 and 20.66 million in 2014–2015, and mortality and chronic bronchitis shared about 93.3% of the total DALYs for PM10. During this period, the economic cost of health impact due to PM10 is approximately US$304,122 million, which accounts for about 2.94% of China’s gross domestic product (GDP). Megacities are expected to contribute relatively more to the total costs. The present methodology could be used as a tool to help policy makers and pollution control board authorities, to further analyze costs and benefits of air pollution management programs in China.