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The increase in atmospheric N2O observed over the last century reflects large-scale human perturbations to the global nitrogen cycle. High-precision measurements of atmospheric N2O over the last decade reveal subtle signals of interannual variability (IAV) superimposed upon the more prominent growth trend. Anthropogenic sources drive the underlying growth in N2O, but are probably too monotonic to explain most of the observed IAV. The causes of both seasonal and interannual variability in atmospheric N2O are explored on the basis of comparisons of a 1993–2004 atmospheric transport simulation to observations of N2O at five stations of the Advanced Global Atmospheric Gases Experiment (AGAGE). The complementary tracers chlorofluorocarbons (CFCs) 11 and 12 and SF6 also are examined. The model simulation does not include a stratospheric sink and thus isolates the effects of surface sources and tropospheric transport. Both model and observations yield correlations in seasonal and interannual variability among species, but only in a few cases are model and observed variability correlated to each other. The results suggest that tropospheric transport contributes substantially to observed variability, especially at Samoa station. However, some features of observed variability are not explained by the model simulation and appear more consistent with a stratospheric influence. At Mace Head, Ireland, N2O and CFC growth rate anomalies are weakly correlated to IAV in polar winter lower stratospheric temperature, a proxy for the strength of the mean meridional stratospheric circulation. Seasonal and interannual variability in the natural sources of N2O may also contribute to observed variability in atmospheric N2O.