Global estimates indicate that agroforestry provides the largest opportunity for agricultural carbon sequestration, while simultaneously delivering diverse benefits to farmers and society, placing it among the most promising natural climate solutions (NCS). Policy and financial actions to support a transition to agroforestry are predicated on the ability to consistently identify agroforestry systems, estimate their carbon benefits, and monitor them over time. However, our review finds critical gaps in each of these areas: climate-positive agroforestry is poorly defined, mitigation estimates are imprecise and use only a fraction of available carbon data, and detection and monitoring are hindered by uncertainty in field and remote-sensing data. To pave the path from theory to practice, we refine standard agroforestry definitions to the subset of agroforestry NCS practices, highlight underappreciated opportunities for agroforestry expansion, and identify avenues to leverage existing data and emerging techniques to predict, map, measure, and track agroforestry's contribution to climate progress.