Net primary production and the flux of dry matter and nutrients from vegetation to soils has increased following four years of exposure to elevated CO2 in a southern pine forest in NC, USA. This has increased the demand for nutrients to support enhanced rates of NPP and altered the conditions for litter decomposition on the forest floor. We quantified the chemistry and decomposition dynamics of leaf litter produced by five of the most abundant tree species in this ecosystem during the third and fourth growing seasons under elevated CO2. The objectives of this study were to determine (i) if there were systemic or species-specific changes in leaf litter chemistry associated with a sustained enhancement of plant growth under elevated CO2; and (ii) whether the process of litter decomposition was altered by increased inputs of energy and nutrients to the forest floor in the plots under elevated CO2. Leaf litter chemistry, including various C fractions and N concentration, was virtually unchanged by elevated CO2. With few exceptions, plant litter produced under elevated CO2 lost mass or N at the same relative rate as that produced under ambient CO2. The relationship between initial litter chemistry and decomposition was not altered by elevated CO2. The greater forest floor mass and nutrient content in the plots under elevated CO2 had no consistent or long-term effect on litter decomposition. Thus, we found no evidence that plant and microbial processes under elevated CO2 resulted in systemic changes in mass loss or N dynamics during decomposition. In contrast to the limited effects of elevated CO2 on litter chemistry and decomposition, there were large differences among species in initial litter chemistry, mass loss and N dynamics during decomposition. If the species composition of this forest community is altered by elevated CO2, the indirect effect of a change in species composition will exert greater control over the long-term rate of nutrient cycling than the direct effect of elevated CO2 on litter chemistry and decomposition dynamics alone.