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Combined PM2.5 and O3 pollution in China has caused negative health impacts on residents and reduced crop yields. The quantitative assessment and prediction of these impacts could provide a scientific basis for policy development. This study assessed the nationwide premature mortality, health effects, and crop damage attributable to PM2.5 and O3 pollution in 2019, and projected the associated health and agricultural losses under a business-as-usual (BAU) scenario for 2025. The economic benefits of improving air quality under different policy scenarios, including the 14th Five-Year Plan (FFP), Secondary Standard Limit (SSL), and Primary Standard Limit (PSL), were also explored. The results showed PM2.5 pollution in 2019 resulted in 246,000 all-cause premature deaths and the economic health loss was RMB 196.509 billion. Similarly, O3 pollution caused 186,300 premature deaths and the economic health loss was RMB 155.807 billion. O3 pollution has led to a loss of 28.5241 million tonnes of crop production and an economic loss of RMB 62.268 billion. Compared with 2019, the avoidable premature deaths from PM2.5 under different scenarios in 2025 were 50,600, 43,000, and 200,300 cases, respectively, exceeding the number of avoided premature deaths from O3 pollution. Compared with the BAU, reducing PM2.5 under different scenarios could generate economic benefits of RMB 70.178 billion, RMB 60.916 billion, and RMB 229.268 billion. Furthermore, the FFP scenario outperformed the SSL in mitigating winter wheat production losses caused by O3 pollution. These results provide important scientific support for the development and evaluation of future comprehensive pollution control measures for PM2.5 and O3. [ABSTRACT FROM AUTHOR]