The terrestrial biosphere sequesters up to a third of annual anthropogenic carbon dioxide emis-sions, offsetting a substantial portion of greenhouse gas forcing of the climate system. Although a number of factors are responsible for this terrestrial carbon sink, atmospheric nitrogen deposition contributes by enhancing tree productivity and promoting carbon storage in tree biomass. Forest soils also represent an important, but understudied carbon sink. Here, we examine the contribution of trees versus soil to total ecosystem carbon storage in a temperate forest and investigate the mechanisms by which soils accumulate carbon in response to two decades of elevated nitrogen inputs. We find that nitrogen-induced soil carbon accumulation is of equal or greater magnitude to carbon stored in trees, with the degree of response being dependent on stand type (hardwood versus pine) and level of N addition. Nitrogen enrichment resulted in a shift in organic matter chemistry and the microbial community such that unfertilized soils had a higher relative abundance of fungi and lipid, phenolic, and N-bearing compounds; whereas, N-amended plots were associated with reduced fungal biomass and activity and higher rates of lignin accumulation. We conclude that soil carbon accumulation in response to N enrichment was largely due to a suppression of organic matter decomposition rather than enhanced carbon inputs to soil via litter fall and root production.