Growing bioenergy crops such as Miscanthus has the potential to mitigate atmospheric carbon dioxide emissions by the replacement of fossil fuels and by storing carbon (C) in the soil due to land use change. Here we compare direct measurements of soil organic C fractions made in Carlow (Ireland) to model predictions made by RothC and a cohort model. Our results show that when Miscanthus is grown on land previously under arable agriculture, the soil organic C will increase to a level above that of native pasture, as Miscanthus organic material is shown to have a slow decomposition rate. In addition we demonstrate that for measured organic C, fractions of different lability are similar to the C pools used in RothC. Using the model predictions from RothC and Miscanthus yields from MISCANFOR, we predict that in Ireland, changing the land use from arable to Miscanthus plantations has the potential to store between 2 and 3 Mg C ha−1 y−1 depending on the crop yield and the initial soil organic C level.