Exposure to ambient ozone (O3) is a risk factor for public health and causes damage to vegetation, including agricultural crops. In this study, we performed a comprehensive estimate of the spatial distribution of premature deaths and main crop yield losses attributed to ambient O3, across China in 2014, by applying the Global Burden of Diseases approach and AOT40 metric (i.e., above a threshold of O3 concentration of 40 ppb). Our results show that China's total premature deaths in 2014 due to COPD attributed to O3 exposure were 89,391 (CI95: 32,225–141,649) with spatial variation across provinces. O3 induced production losses from all crops were 78.4 million metric tons, and the relative yield losses ranged from 8.5 to 14.0% for winter wheat, 3.9–15.0% for rice, and 2.2–5.5% for maize. The top four Chinese provinces (Sichuan, Shandong, Henan and Hunan) for premature deaths attributed to O3 pollution also suffered severe losses in yields of winter wheat and rice. Our results provide quantitative evidence of O3 induced impacts on both the public health and crop yields across Chinese provinces, which have important policy implications for the government to alleviate O3 pollution in addition to PM2.5 pollution that is currently being addressed.