The Earth is at a critical juncture, facing the existential threat of climate change and an urgent need for sustainable solutions. This chapter synthesizes current information on the link between agroforestry, climate change, and carbon (C) sequestration, highlighting the potential of agroforestry as a natural climate solution. Agroforestry systems (AFS) act as C sinks, absorbing significant amounts of atmospheric carbon dioxide (CO2) through tree growth and long-term storage in biomass and soils. Agroforestry helps offset greenhouse gas emissions by increasing C sequestration, contributing to global efforts to lower atmospheric CO2 levels and mitigate climate change. Globally, AFS has the potential to remove 0.1–5.7 billion tons of CO2 from the atmosphere each year, while storing more than 36 billion tonnes of C above and below ground. Among different AFS, improved fallows are more effective in aboveground C sequestration (11.29 tC ha−1 yr−1), while silvopastoral systems are more efficient for soil C sequestration (4.38 tC ha−1 yr−1). Adopting agroforestry can significantly contribute to the sustainability and resilience of our planet’s future. Despite its inclusion in global climate policy agreements, agroforestry has been slow to implement. Increasing adoption requires a collective effort from governments, organizations, farmers, and communities.