Increasing air pollution, particularly in terms of fine particulate matter (PM2.5) and ozone (O3), caused by large-scale fossil fuel combustion, affects human health and economic activities in China. In this study, we analyzed the spatiotemporal trends of carbon emissions, carbon emission intensity, and concentrations of PM2.5 and O3 in 30 provincial-level administrative regions of China during 2010–2019. Overall, an increasing trend was observed in carbon emissions, with high emissions occurring in Shandong, Hebei, and Jiangsu in particular. The highest growth rates of carbon emissions were 169% and 117% in Xinjiang and Ningxia, respectively. Conversely, the carbon emission intensities and concentrations of PM2.5 and O3 decreased across the study regions at different rates. The western and central regions experienced the greatest decrease in carbon emissions in 2019 compared with that of 2010, followed by those in the northeastern and eastern regions. Spatiotemporal variations suggest that pollution control is essential for improving air quality and offsetting the negative impact of increased energy consumption. Overall, this study shows that pollution control policies lead to short-term improvements in air quality, and hence that the implementation of stringent environmental protection policies is essential.