The expansion of agroforestry could provide substantial climate change mitigation (up to 0.31 Pg C yr−1), comparable to other prominent natural climate solutions such as reforestation. Yet, climate-focused agroforestry efforts grapple with ambiguity about which agroforestry actions provide mitigation, uncertainty about the magnitude of that mitigation and inability to reliably track progress. In this perspective, we define agroforestry as a natural climate solution, discuss current understanding of the controls on farm-scale mitigation potential and highlight recent innovation on emergent, high-resolution remote sensing methods to enable detection, measurement and monitoring. We also assess the status of agroforestry in the context of global climate ambitions, highlighting regions of underappreciated expansion opportunity and identifying priorities for policy and praxis.