With the continuous advancement of urbanization and industrialization, non-grain production on cropland (NGPCL) is gradually becoming more widespread. This phenomenon will compress the space for grain production and trigger a global food crisis. How to scientifically understand and effectively control NGPCL has become a scientific issue. This study, conducted at the plot scale, establishes a measurement index for NGPCL and further explores the characteristics and driving mechanisms of NGPCL in mountainous areas. The results indicate the following: (1) Compared to plots for food-growing, plots for non-grain production tend to be more dispersed, with terraces showing the most significant dispersion, while plains exhibit the highest degree of aggregation. (2) In terms of irrigation conditions, irrigated land and dry land are more likely to undergo NGPCL. In terms of topography, slope croplands have the highest probability of being used for NGPCL. (3) Regions with steeper slopes, higher elevations, greater differences in altitude from the settlement, farther distances from settlements and roads, yet closer proximity to forests, are more likely to engage in NGPCL. (4) Different plot characteristics have varying impacts on NGPCL. Plot characteristics primarily affect the costs and returns of grain production, driving farmers to change their production patterns and triggering NGPCL.