With frequent severe haze and smog episodes in Chinese cities, an increasing number of studies have focused on estimating the impact of fine particulate matter (PM2.5)on public health. However, the current use of national and provincial demographic data might mask regional differences and lead to inaccurate estimations of pollution-related health impacts across cities. We applied the Global Burden of Disease methodology to develop a dataset of premature deaths attributed to ambient PM2.5 in 129 Chinese cities in 2006, 2010 and 2015, based on the information of baseline mortality rates and population densities at the city level. Our results suggested that ambient PM2.5 pollution led to 631,230 (95% confidence interval: 281,460–873,800)premature deaths in those cities in 2015, which was similar to that in 2010, but 42.8% higher than that in 2006. The reduction of premature deaths was not as obvious as the improvement in air quality in recent years, primarily owing to the aging Chinese population. For large and medium/small cities, the effects of PM2.5 abatement on alleviating public health burdens were lower than those for megalopolises and metropolises; however, such large and medium/small cities are at risk of increasing future PM2.5 pollution levels due to rapid development. Significant differences in PM2.5-induced premature deaths indicated the need for specific policies to mitigate the health burden of air pollution in different types of Chinese cities.