Synergizing air pollution control and climate change mitigation has been of significant academic and policy concern. The synergy between air pollution and carbon emissions is one of the measures to understand the characteristics and process of the air pollution–carbon synergistic control, which will also provide valuable information for collaboratively achieving Sustainable Development Goals (SDGs) (such as SDGs 11 and 13). This study establishes a systematic framework integrating emissions inventory and projection models, correlation mining and typology analysis methods to predictively evaluate the synergy and comprehensive coordination between air pollution and carbon dioxide (CO2) emissions in Chinese cities by 2030, 2050, and 2060 under different policy scenarios for air pollution and CO2 emissions control. The results reveal the significant effects of synergistically implementing clean air and aggressive carbon-reducing policies on mitigating air pollution and CO2 emissions. Under the On-time Peak-Net Zero-Clean Air and Early Peak-Net Zero-Clean Air scenarios, the total reduction and synergy for air pollution and CO2 emissions will be more significant, particularly by 2050 and 2060. This study is the first to integrate scenario projection and synergy evaluation in air pollution and CO2 research, providing a novel supplement to the air pollution–climate change synergy methodology based on co-benefit estimation. The methods and findings will also contribute to measuring the achievement and analyzing the interaction of the SDGs.