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The improvement of grain processing capacity is crucial to the realization of grain security. Enterprises are important grain processing bodies and their productivity directly determines grain processing capacity. Chinese grain processing enterprises still have difficulties, and how to further improve grain processing capacity and the total factor productivity of grain processing enterprises may be an important aspect. We used the meta-frontier Malmquist index to measure the total factor productivity of grain enterprises as well as judge the change trend and regional gap, applying the classical regression model to test the convergence of China’s overall and regional grain enterprises’ total factor productivity. This research finds that the total factor productivity of grain processing enterprises increased by 1.18% annually during the sample period, and that of the central region rose more quickly than the other areas of China. Technical progress contributes more to enterprises’ total factor productivity, but technical efficiency may become a key factor in determining it. The difference in the growth rate of the grain processing enterprises’ total factor productivity among different ones in the eastern and western regions is gradually narrowing, while that of the central region is gradually expanding; there is an obvious technological catch-up effect between and within the regions, especially in the central area of China.