Increasing global demand for agricultural commodities spurs conversions of natural ecosystems. Sustainable intensification in areas of high yield gaps has been proposed a pathway to achieve food security, support rural livelihoods, while also reducing the impact of commodity production by narrowing yield gaps on existing agricultural lands, while improving resource efficiency. Following the dissolution of the Union of Soviet Socialist Republics (USSR), Georgia experienced one of the highest losses of agricultural productivity among all former USSR countries and is now highly dependent on food imports. Closing yield gaps in Georgia through sustainable intensification has the potential to increase food self-sufficiency, support rural livelihoods, and strengthen food security and sovereignty. We estimated its potential for sustainable intensification in current agricultural areas to achieve self-sufficiency for wheat, maize, and barley. We found that crop yields can be doubled to tripled under high-input production systems, using high-yielding varieties, optimized inputs, fertilizers, and pest control. Yet, self-sufficiency in wheat can only be reached if at least 80% of the potentially attainable yields are achieved and if land is strategically allocated between crops. To achieve such increases, farmers need access to and training for using different crop varieties, fertilizers, and pest and disease control practices and products. Intensification increases the risks to ecosystem services’ health and livelihoods, particularly raising equity concerns. Yet, intensifying very low input systems is often found to be more sustainable, with high yield increases compared to limited impacts on the environment. The high employment rate in the agricultural sector in Georgia particularly provides opportunities to reduce poverty and increase livelihoods through increasing incomes and food security.