Abstract: In recent years, the intensification of the trend of “non-grain” cultivated land has not only increased China’s dependence on external food resources but has also placed greater pressure on maintaining high levels of grain production in the future. Because of the ongoing expansion of the social and economic sectors and the growth of non-agricultural industries, the relocation of rural populations from primary to secondary and tertiary occupations has become a prevalent phenomenon. Most studies have focused on the impact of the broader phenomenon of non-agricultural labor transfer on the cropping structure. However, this approach fails to consider that labor transfer is not merely an individual decision but rather an adjustment of the household’s resource allocation strategy. The transfer of labor from agricultural to non-agricultural sectors will not only affect the allocation of labor within households but also alter the structure of household income, thus creating differences in both labor allocation and financial resources. Considering the these factors, this study employs data from 3 709 farming households nationwide to examine the impact of non-agricultural transfer of labor on grain cultivation. The study takes into account shifts in the distribution of household labor and income structure and explores the mechanism of non-agricultural transfer of labor on grain cultivation from the perspectives of agricultural socialization services, agricultural machinery use, and land transfer. Moreover, this analysis considers the impact of regional heterogeneity. The average ratio of grain-cultivated area to total cultivated area in the samples was 49%, the average ratio of non-agricultural labor force to total household labor was 25%, and the average ratio of non-agricultural income to total household income was 76%. Additionally, the transfer of labor from agricultural to non-agricultural sectors altered the structure of income and employment for agricultural households. This, in turn, influenced the decision-making process regarding grain cultivation as households sought to purchase agricultural socialization services, adopt agricultural machinery, and transfer land. Moreover, the impact of the non-agricultural transfer of labor varied among different grain-producing areas. The promotion of grain cultivation was more pronounced in villages situated in non-suburban or non-plain areas. Considering the specific circumstances of agricultural households and prevailing conditions of grain production in each region is essential. This will ensure the formulation of targeted policy measures that can effectively address the challenges posed by labor force transfer, changes in income structure, and other factors. Such measures are crucial for maintaining food security in China and promoting increased production and income of agricultural households.