China has successfully reduced particulate matter pollution, but ozone concentrations continually grow. Here, we employed a atmospheric chemistry-climate model and modified two crop models with considering the effects of diffuse fertilization and ozone, which were validated by multiple observations. Using the state-of-the-art modeling approach, we assess effects of ozone and aerosols on rice and wheat under two contrasting air pollution emission scenarios in China, rigorous emission controls versus current legislation. Currently, ozone and aerosol pollution together induces 11.3% yield losses for rice and 14.6% for wheat. Following the current legislation scenario, we simulate additional yield declines of 5.4% for rice and 0.4% for wheat. However, implementation of maximum feasible technological reductions in emissions relative to the current legislation scenario avoids rice and wheat yield losses by 14–15%, economically equivalent to 18.9 billion USD. Such remarkable benefits are primarily from ozone controls, whose mitigating effect is approximately double that of the aerosol reductions. This demonstrates that reprioritizing air pollution control targets from particulate aerosols alone to both aerosols and ozone can substantially alleviate crop losses in China.