This study highlights the significant potential for agroforestry expansion in Jharkhand State, India, as a means to advance multiple Sustainable Development Goals (SDGs), including poverty reduction, biodiversity conservation, and climate change mitigation. Using geographic information system (GIS) modeling, researchers assessed land suitability for agroforestry at the district level, incorporating climate (temperature and precipitation), topography (slope and elevation), ecology (tree cover and normalized difference vegetation index (NDVI)), and socio-economic factors (poverty rate and tribal dominance). The findings indicate that six districts—Simdega (78.20%), Pakur (76.25%), West Singhbhum (72.70%), Dumka (68.84%), Sahibganj (64.63%), and Godda (63.43%)—possess agroforestry potential exceeding 60%. Additionally, 513 villages were identified as highly suitable (≥80%) for agroforestry, offering opportunities to improve livelihoods among marginalized communities. Outside forested areas, 8.58% of Jharkhand’s total land is classified as wasteland, much of which is viable for agroforestry practices. Implementing agroforestry in these areas could sequester 637 tons of carbon annually while generating economic benefits for local populations and contributing to carbon emission reduction efforts. Given Jharkhand’s abundant high-potential land, the study emphasizes the need for village-level agroforestry adoption as a priority. It also calls for policy attention and investment to support agroforestry expansion, which could help achieve 9 out of the 17 SDGs.