The coupled terrestrial biogeochemical cycles of silicon (Si) and carbon (C) that are driven by plant action play a crucial role in the regulation of atmospheric CO 2 . Generally, the processes involved in the coupled cycles of Si and C include plant-enhanced silicate weathering, phytolith formation and solubilization, secondary aluminosilicate accumulation, phytolith occlusion of C as well as physico-chemical protection of organic C in soils. There is increasing evidence of biological pumping of Si in terrestrial ecosystems, suggesting that complex feedbacks exist amongst the processes within the coupled Si and C cycles. Recent advances in the coupled Si and C cycles offer promising new possibilities for enhancing atmospheric CO 2 sequestration. Organic mulching, rock powder amendment, cultivating Si-accumulating plants and partial plant harvesting are potential measures that may allow for long-term manipulation and biogeochemical sequestration of atmospheric CO 2 in soil–plant systems.