More than half of the world’s population is nourished by crops fertilized with synthetic nitrogen (N). However, N fertilization is a major source of anthropogenic emissions, augmenting the carbon footprint (CF). To date, no global quantification of the CF induced by N fertilization of the main grain crops has been performed, and quantifications at the national scale have neglected the CO₂ assimilated by plants. A first Cradle-Grave life cycle assessment was performed to quantify the CF of the N fertilizers’ production, transportation, and application to the field and the uses of the produced biomass in livestock feed, human food, and biofuel production. We quantified direct and indirect inventories emitted or sequestered by the N fertilization of grain crops (wheat, maize, and rice). Grain food produced with N fertilization had a net CF of 7.4 Gt CO₂eq. in 2019 after excluding the assimilated C in plant biomass, which accounted for a quarter of the total CF. The Cradle (fertilizer production and transportation), Gate (fertilizer application, and soil and plant systems), and Grave (feed, food, biofuel, and losses) stages contributed to the CF by 2, 11, and 87%, respectively. Although Asia was the top grain producer, North America contributed 38% of the CF due to the greatest CF of the Grave stage (2.5 Gt CO₂eq.). The CF of grain crops will increase to 21.2 Gt CO₂eq. in 2100, driven by the rise in N fertilization to meet the growing food demand without actions to stop the decline in N use efficiency. To meet the targets of climate change, we introduced an ambitious mitigation strategy, including the improvement of N agronomic efficiency (6% average target for the three crops) and manufacturing technology, reducing food losses, and global conversion to healthy diets, whereby the CF can be reduced to 5.6 Gt CO₂eq. in 2100.