Abstract: Increasing grain production while protecting the environment is an important prerequisite for ensuring sustainable development and food security of China. To explore effective strategies to improve the ecology total factor productivity of grain (ETFP) in China, this study used the Global-Malmquist-Luenberger (GML) index to measure the ETFP based on the ecological value of grain production. Based on the theory of public goods, we empirically explored the path to improve ETFP with agricultural infrastructure as the point of penetration. We found: (1) The ecological value of grain production per hectare in 30 provinces (cities, autonomous regions) of China increased from 1993 to 2019. The average ETFP during 1993–2019 generally showed a fluctuating upward trend. Among them, the ETFP of the Middle and Lower Reaches of the Yangtze River and the Northeast China were higher than the national average in most years. (2) Agricultural water conservancy facilities, agricultural electric power facilities, and agricultural transportation facilities can effectively improve ETFP, but there was a lag in time. Among these factors, the impact of agricultural water conservancy facilities on ETFP showed an “inverted U” shape. This finding suggests that there is an optimum value for the provision of agricultural field water conservancy facilities in the process of ecological food production. (3) In contrast to the full-sample regression results, the regression results of samples of northern and southern regions showed that the agricultural water conservancy facilities and their lag terms had no significant impact on ETFP, and the agricultural electric power facilities and their lag terms had a reducing effect on ETFP in southern region. The results of the sample regression showed that agricultural electric facilities and their lag items in main grain-producing areas had no significant impact on ETFP, while agricultural electric power facilities and their lag items in non-main grain-producing areas had no significant impact on ETFP. (4) The results of the moderating effect test indicated that environmental regulation had a positive moderating effect on ETFP. Further study found that, in the grouping regulation regression results, environmental regulation could play a stronger positive regulatory role in the region with a lower ETFP than in the region with a higher ETFP. Therefore, on the basis of this research, we recommend that the government should plan and invest in agricultural infrastructure construction in advance and formulate and publicize scientific, reasonable, and flexible environmental laws and regulations. This study innovatively incorporates the ecological value of grain production into the measurement of ETFP. While broadening the research boundary of agricultural infrastructure construction planning, it provides a basis for improving the ETFP in China.