<p>Intercropping, the simultaneous cultivation of multiple crops, enhances resource efficiency and biodiversity while reducing greenhouse gas emissions (GHGE) compared to monoculture systems. This review assesses intercropping’s potential to mitigate GHGE (reductions of 15–25%) and increase yields (20–40%) across diverse agroecosystems. It emphasizes the need for tailored management strategies and region-specific research to overcome adoption barriers and optimize intercropping for sustainable agriculture. However, these benefits vary significantly by region, crop combination, climate, and management practices, with limitations and trade-offs discussed in detail in this review. A systematic review of 1,356 articles from databases like Google Scholar, Scopus, and Web of Science was conducted, with 95 studies selected for detailed analysis. The focus was on empirical evidence highlighting intercropping’s impact on GHGE, mechanisms such as nitrogen fixation, and regional variations in implementation. Intercropping, particularly with leguminous crops, significantly reduces CO₂ emissions by enhancing biological nitrogen fixation, reducing synthetic fertilizer use, and improving soil fertility. Diverse root systems in intercropping systems promote nutrient cycling, soil structure, and microbial activity, leading to better organic matter decomposition and nutrient availability. However, adoption barriers, including economic constraints and environmental factors, vary regionally, necessitating tailored management strategies. Intercropping offers a viable strategy for balancing agricultural productivity and ecological sustainability by mitigating GHGE and enhancing food security. This review highlights the need for region-specific research and actionable strategies to overcome adoption barriers and optimize intercropping systems for global agricultural sustainability.</p>