Nitrogen deposition rates in southern California are the highest in North America and have had substantial effects on ecosystem functioning. We document changes in the belowground C cycle near ponderosa pine trees experiencing experimental nitrogen (N) addition (50 and 150 kg N ha−1 a−1 as slow release urea since 1997) at two end-member sites along a pollution gradient in the San Bernardino Mountains, California. Despite considerable differences in N deposition between the two sites, we observed parallel changes in microbial substrate use and soil enzyme activity with N addition. Δ14C measurements indicate that the mean age of C respired by the Oa horizon declined 10–15 years with N addition at both sites. N addition caused an increase in cellulolytic enzyme activity at the polluted site and a decrease in ligninolytic enzyme activity at the unpolluted site. Given the likely differences in lignin and cellulose ages, this could explain the difference in the age of microbial respiration with N addition. Measurements of fractionated soil organic matter did not show the same magnitude of changes in response to N addition as were observed for respired C. This lesser response was likely because the soils are mostly composed of C having turnover times of decades to centuries, and 9 years of N amendment were not enough to affect this material. Consequently, Δ14C of respired CO2 provided a more sensitive indicator of the effects of N addition than other methods. Results suggest that enhanced N deposition alone may not result in increased soil C storage in xeric ecosystems.