AbstractNational scale projections of bioenergy crop yields and their environmental impacts are essential to identify appropriate locations to place bioenergy crops and ensure sustainable land use strategies. In this study, we used the process‐based Daily Century (DAYCENT) model with site‐specific environmental data to simulate sorghum (Sorghum bicolor L. Moench) biomass yield, soil organic carbon (SOC) change, and nitrous oxide emissions across cultivated lands in the continental United States. The simulated rainfed dry biomass productivity ranged from 0.8 to 19.2 Mg ha−1 year−1, with a spatiotemporal average of  Mg ha−1 year−1, and a coefficient of variation of 35%. The average SOC sequestration and direct nitrous oxide emission rates were simulated as  Mg CO2e ha−1 year−1 and  Mg CO2e ha−1 year−1, respectively. Compared to field‐observed biomass yield data at multiple locations, model predictions of biomass productivity showed a root mean square error (RMSE) of 5.6 Mg ha−1 year−1. In comparison to the multi State (n = 21) NASS database, our results showed RMSE of 5.5 Mg ha−1 year−1. Model projections of baseline SOC showed RMSE of 1.9 kg/m2 in comparison to a recently available continental SOC stock dataset. The model‐predicted N2O emissions are close to 1.25% of N input. Our results suggest 10.2 million ha of cultivated lands in the Southern and Lower Midwestern United States will produce >10 Mg ha−1 year−1 with net carbon sequestration under rainfed conditions. Cultivated lands in Upper Midwestern states including Iowa, Minnesota, Montana, Michigan, and North Dakota showed lower sorghum biomass productivity (average: 6.9 Mg ha−1 year−1) with net sequestration (average: 0.13 Mg CO2e ha−1 year−1). Our national‐scale spatially explicit results are critical inputs for robust life cycle assessment of bioenergy production systems and land use‐based climate change mitigation strategies.