The rates of carbon bio-sequestration within silica phytoliths of the leaf litter of 10 economically important bamboo species indicates that (a) there is considerable variation in the content of carbon occluded within the phytoliths (PhytOC) of the leaves between different bamboo species, (b) this variation does not appear to be directly related to the quantity of silica in the plant but rather the efficiency of carbon encapsulation by the silica. The PhytOC content of the species under the experimental conditions ranged from 1.6% to 4% of the leaf silica weight. The potential phytolith carbon bio-sequestration rates in the leaf-litter component for the bamboos ranged up to 0.7 tonnes of carbon dioxide (CO2) equivalents (t-e-CO2) ha−1 yr−1 for these species. Assuming a median phytolith carbon bio-sequestration yield of 0.36 t-e-CO2 ha−1 yr−1, the global potential for bio-sequestration via phytolith carbon (from bamboo and/or other similar grass crops) is estimated to be ∼1.5 billion t-e-CO2 yr−1, equivalent to 11% of the current increase in atmospheric CO2. The data indicate that the management of vegetation such as bamboo forests to maximize the production of PhytOC has the potential to result in considerable quantities of securely bio-sequestered carbon.