In this paper we establish a model that expresses the coupled relationship between grain yield and agricultural labor changes in China, and present a preliminary discussion of the coupled processes involved in changes in these factors at the county level. Thus, we develop two coefficients on the basis of county-level statistical data for grain yield and agricultural labor for the years 1991, 2000, and 2010, namely, the grain-labor elasticity coefficient(GLEC) and the agricultural labor-transfer effect coefficient(ALTEC). The results of this study show that during the transformation process of agricultural development in China, different kinds of coupled relationships between grain yield and agricultural labor changes co-existed at the same time. For example, between 1991 and 2010, counties characterized by three different coupled modes(i.e., increasing grain yield and decreasing agricultural labor, increasing grain yield and agricultural labor, and decreasing grain yield and agricultural labor) account for 48.85%, 29.11%, and 19.74% of the total across the study area, respectively. Interestingly, a coupled relationship between increasing grain yield and decreasing agricultural labor is mainly concentrated in the traditional farming areas of China, while a coupled relationship between increasing grain yield and agricultural labor is primarily concentrated in pastoral areas and agro-pastoral ecotones in underdeveloped western China. At the same time, a coupled relationship between decreasing grain yield and agricultural labor is concentrated in areas that have experienced a rapid development transition in agriculture, especially the developed southeastern coast of China. The results of this study also show that between 1991 and 2010, 1961 counties experienced a decline in the proportion of agricultural labor; of these, 1452 are also characterized by increasing grain yield, 72.38% of the total. This coupled relationship between grain yield and changes in the proportion of agricultural labor shows a stepped fluctuation and has continually strengthened over time. Data show that mean values for the GLEC and ALTEC increased from –0.25 and –2.93 between 1991 and 2000 to –0.16and –1.78 between 2000 and 2010, respectively. These changes in GLEC and ALTEC illustrate that the influence of agricultural labor changes on increasing grain yields has gradually diminished. Finally, the results of this study reveal that the ‘Hu Huanyong Line’ is a significant boundary sub-dividing this coupled relationship between grain yield and changes in agricultural labor.