Recent research has dramatically advanced our understanding of soil organic matter chemistry and the role of N in some organic matter transformations, but the effects of N deposition on soil C dynamics remain difficult to anticipate. We examined soil organic matter chemistry and enzyme kinetics in three size fractions ([250 lm, 63-250 lm, and \63 lm) following 6 years of simulated atmospheric N deposition in two ecosystems with contrasting litter biochemistry (sugar maple, Acer saccharum-basswood, Tilia americana and black oak, Quercus velutina-white oak, Q. alba). Ambient and simulated (80-kg NO 3 --N ha -1 year -1 ) atmospheric N deposition were studied in three replicate stands in each ecosystem. We found striking, ecosystem-specific effects of N deposition on soil organic matter chemistry using pyrolysis gas chromatography/mass spectrometry. First, furfural, the dominant pyrolysis product of polysaccharides, was significantly decreased by simulated N deposition in the sugar maple-basswood ecosystem (15.9 vs. 5.0%) but was increased by N deposition in the black oak-white oak ecosystem (8.8 vs. 24.0%). Second, simulated atmospheric N deposition increased the ratio of total lignin derivatives to total polysaccharides in the [250 lm fraction of the sugar maple-basswood ecosystem from 0.9 to 3.3 but there were no changes in other size classes or in the black oak-white oak ecosystem. Third, simulated N deposition increased the ratio of lignin derivatives to N-bearing compounds in the 63-250 and [250 lm fractions in both ecosystems but not in the \63 lm fraction. Relationships between enzyme kinetics and organic matter chemistry were strongest in the particulate fractions ([63 lm) where there were multiple correlations between oxidative enzyme activities and concentrations of lignin derivatives and between glycanolytic enzyme activities and concentrations of carbohydrates. Within silt-clay fractions (\63 lm), these enzyme-substrate correlations were attenuated by interactions with particle surfaces. Our results demonstrate that variation in enzyme activity resulting from atmospheric N deposition is directly linked to Electronic supplementary material The online version of this article (