Growing cellulosic feedstock crops (e.g., switchgrass) for biofuel is more environmentally sustainable than corn-based ethanol. Specifically, this practice can reduce soil erosion and water quality impairment from pesticides and fertilizer, improve ecosystem services and sustainability (e.g., serve as carbon sinks), and minimize impacts on global food supplies. The main goal of this study was to identify high-risk marginal croplands that are potentially suitable for growing cellulosic feedstock crops (e.g., switchgrass) in the US Great Plains (GP). Satellite-derived growing season Normalized Difference Vegetation Index, a switchgrass biomass productivity map obtained from a previous study, US Geological Survey (USGS) irrigation and crop masks, and US Department of Agriculture (USDA) crop indemnity maps for the GP were used in this study. Our hypothesis was that croplands with relatively low crop yield but high productivity potential for switchgrass may be suitable for converting to switchgrass. Areas with relatively low crop indemnity (crop indemnity <$2 157 068) were excluded from the suitable areas based on low probability of crop failures. Results show that approximately 650 000 ha of marginal croplands in the GP are potentially suitable for switchgrass development. The total estimated switchgrass biomass productivity gain from these suitable areas is about 5.9 million metric tons. Switchgrass can be cultivated in either lowland or upland regions in the GP depending on the local soil and environmental conditions. This study improves our understanding of ecosystem services and the sustainability of cropland systems in the GP. Results from this study provide useful information to land managers for making informed decisions regarding switchgrass development in the GP.