Changes in land use and management practices to store and sequester carbon are becoming integral to global efforts that both address climate change and alleviate poverty. Knowledge and evidence gaps nevertheless abound. This paper analyses the most pressing deficiencies in understanding carbon storage in both soils and above ground biomass and the related social and economic challenges associated with carbon sequestration projects. Focusing on the semi-arid and dry sub-humid systems of sub-Saharan Africa which are inhabited by many of the world’s poor, we identify important interdisciplinary opportunities and challenges that need to be addressed, in order for the poor to benefit from carbon storage, through both climate finance streams and the collateral ecosystem service benefits delivered by carbon-friendly land management. We emphasise that multi-stakeholder working across scales from the local to the regional is necessary to ensure that scientific advances can inform policy and practice to deliver carbon, ecosystem service and poverty alleviation benefits.