Household consumption in China is associated with substantial PM2.5 pollution, through activities directly (i.e., fuel use) and/or indirectly (i.e., consumption of goods and services) causing pollutant emissions. Urban and rural households exhibit different consumption preferences and living areas, thus their contributions to and suffering from air pollution could differ. Assessment of this contrast is important to understand the environmental impacts of the nation’s ongoing urbanization process. Here we quantify Chinese urban and rural households’ contributions to ambient PM2.5 pollution and the health risks they suffer from, by integrating economic, atmospheric, and health models and/or datasets. The national premature deaths related to long-term exposure to PM2.5 pollution contributed by total household consumption are estimated to be 1.1 million cases in 2015, among which 56% are urban households and 44% are rural households. For pollution contributed indirectly, urban households, especially in developed provinces, tend to bear lower mortality risks compared with the portions of deaths or pollution they contribute. The opposite results are true for direct pollution. With China’s rapid urbanization process, the increased indirect pollution-associated premature deaths could largely offset that avoided by reduced direct pollution, and the indirect pollution-associated urban-rural inequalities might become severer. Pollution mitigation strategies from both production and consumption sides could be developed to reduce pollution-related mortality and associated urban-rural inequality.