Agroforestry is a land-use system where woody perennials are deliberately combined with agricultural crops and/or livestock on the same land-management units in some form of spatial arrangement or temporal sequence. Agroforestry has the potential to respond to multiple challenges related to soil carbon sequestration including soil fertility improvement, land restoration, food security and adaptation and resilience to climate change. In this chapter, we show how agroforestry systems (AFSs) address several of the above-mentioned challenges, and play a key role in boosting soil carbon sequestration (SCS) and improving soil functions. Other co-benefits are also considered, i.e., soil and ecosystem services, and the wellbeing of rural populations (increase in income, access to non-timber products, etc.), mainly in the less developed countries. Attention is also paid to the main barriers, which may lessen or halt SCS in AFSs. We make recommendations for implementing and improving AFSs to foster SCS and to meet the challenges faced by human societies in the 21st century.