Producing enough food within environmental limits has faced severe challenges in recent years. Enhancing resource utilization and reducing environmental emissions are two important aspects in addressing these challenges. However, there is a lack of systematic reflection of the environmental sustainability in food production that integrates both the EFF and the planetary boundaries, particularly concerning the specific distinction between the environmental sustainability of resource utilization and environment emissions. This study developed an approach to integrate environmental footprint family and planetary boundaries for assessing the environmental sustainability in food production. Additionally, key responses from the aspects of resource uses and environmental emissions have also been identified. The approach was applied to assess the environmental sustainability in China's grain production, which has recently been prioritized as a primary development goal in its agricultural development. The results indicated an improvement in the environmental sustainability of China's grain production since 2015, and the grain sustainability index increased from 0.77 to 0.81. Moreover, implications for key responses to improve the environmental sustainability of food production were also identified. The approach not only assessed the environmental sustainability in food production, but also provided insights to enhance the synergistic security of both food and environment.