Food self-sufficiency has long been regarded as essential for understanding and managing urban and regional food systems; however, few studies have examined the food self-sufficiency of megacity regions within a comprehensive framework that distinguishes different types of agricultural land (i.e., arable land, horticultural landscapes, and waters). To fill these gaps, we took the Pearl River Delta as a case study and quantified the foodsheds of different types of agricultural land by calculating the land footprint of food consumption. On this basis, food self-sufficiency is defined as the ratio of available and required agricultural area for regional food demand. The results indicated that the self-sufficiency level provided by the arable land in the Pearl River Delta is low and cannot realize self-sufficiency at the regional and urban levels. The horticultural landscapes can provide self-sufficiency at the regional level, whereas the regions with water cannot, as their foodsheds extend over the boundary of the Pearl River Delta. For arable land, establishing a localized regional food system requires expanding the foodshed size. These findings provide evidence that megacity regions may face increasing difficulties in achieving self-sufficiency in the near future. This research can improve policymakers’ understanding of the sustainability and resilience of regional food systems in megacity regions.