Terrestrial and oceanic ecosystems contribute almost equally to the sequestration of ca 50 per cent of anthropogenic CO2 emissions, and already play a role in minimizing our impact on Earth’s climate. On land, the majority of the sequestered carbon enters soil carbon stores. Almost one-third of that soil carbon can be found in peatlands, an area covering just 2-3% of the Earth’s landmass. Peatlands are thus well established as powerful agents of carbon capture and storage; the preservation of archaeological artefacts, such as ancient bog bodies, further attest to their exceptional preservative properties. Peatlands have higher carbon storage densities per unit ecosystem area than either the oceans or dry terrestrial systems. However, despite attempts over a number of years at enhancing carbon capture in the oceans or in land-based afforestation schemes, no attempt has yet been made to optimize peatland carbon storage capacity or even to harness peatlands to store externally captured carbon. Recent studies suggest that peatland carbon sequestration is due to the inhibitory effects of phenolic compounds that create an ‘enzymic latch’ on decomposition. Here, we propose to harness that mechanism in a series of peatland geoengineering strategies whereby molecular, biogeochemical, agronomical and afforestation approaches increase carbon capture and long-term sequestration in peat-forming terrestrial ecosystems.