Total crop production is a function of the harvested area and the yield. Many studies have investigated opportunities to increase production by closing the yield gap and by expanding cropland area. However, the potential to increase the harvested area by increasing the cropping frequency on existing cropland has remained largely unexplored. Our study suggests that the attainable harvested area gap (HAG) in China ranges from 13.5 to 36.3 million ha, depending on the selected water allocation scenario, relative to the current harvested area of 160.0 million ha. Spatially, South China and the Lower Yangtze region have the largest potential to increase harvested area, as these regions allow triple-cropping, have sufficient water available, and have a good irrigation infrastructure. The results imply that management factors are equally important for exploring the potential against the resource endowment: water allocation has a large impact on both the size and the spatial pattern of the attainable HAG. This indicates the necessity of further examining the spatial-temporal dynamics of HAG at national and regional scales, and its potential contribution to food security and sustainable agricultural development.