The role of the organic carbon occluded within phytoliths (referred to in this text as 'PhytOC') in carbon sequestration in some soils is examined. The results show that PhytOC can be a substantial component of total organic carbon in soil. PhytOC is highly resistant to decomposition compared to other soil organic carbon components in the soil environments examined accounting for up to 82% of the total carbon in well-drained soils after 1000 years of organic matter decomposition. Estimated PhytOC accumulation rates were between 15 and 37% of the estimated global mean long-term (i.e. on a millenial scale) soil carbon accumulation rate of 2.4 g C m -2 yr -1 indicating that the accumulation of PhytOC within soil is an important process in the terrestrial sequestration of carbon. The rates of phytolith production and the long-term sequestration of carbon occluded in phytoliths varied according to the overlying plant community. The PhytOC yield of a sugarcane crop was 18.1 g C m -2 yr -1, an accumulation rate that is sustainable over the long-term (millenia) and yet comparable to the rates of carbon sequestration that are achievable (but only for a few decades) by land use changes such as conversion of cultivated land to forest or grassland, or a change of tillage practices from conventional to no tillage. This process offers the opportunity to use plant species that yield high amounts of PhytOC to enhance terrestrial carbon sequestration.