Rates of nitrogen (N) deposition have increased in arid and semiarid ecosystems, but few studies have examined the impacts of long-term N enrichment on ecological processes in deserts. We conducted a multiyear, nutrient-addition study within 15 Sonoran Desert sites across the rapidly growing metropolitan area of Phoenix, Arizona (USA). We hypothesized that desert plants and soils would be sensitive to N enrichment, but that these effects would vary among functional groups that differ in terms of physiological responsiveness, proximity to surface N sources, and magnitude of carbon (C) or water limitation. Inorganic N additions augmented net potential nitrification in soils, moreso than net potential N mineralization, highlighting the important role of nitrifying microorganisms in the nitrate economy of drylands. Winter annual plants were also responsive to nutrient additions, exhibiting a climate-driven cascade of resource limitation, from little to no production in seasons of low rainfall (winter 2006 and 2007), to moderate N limitation with average precipitation (winter 2009), to limitation by both N and P in a season of above-normal rainfall (winter 2008). Herbaceous production is a potentially important mechanism of N retention in arid ecosystems, capable of immobilizing an amount equal to or greater than that deposited annually to soils in this urban airshed. However, interannual variability in precipitation and abiotic processes that limit the incorporation of detrital organic matter into soil pools may limit this role over the long term. In contrast, despite large experimental additions of N and P over four years, growth of Larrea tridentata, the dominant perennial plant of the Sonoran Desert, was unresponsive to nutrient enrichment, even during wet years. Finally, there did not appear to be strong ecological interactions between nutrient addition and location relative to the city, despite the nearby activity of nearly four million people, perhaps due to loss or transfer pathways that limit long-term N enrichment of ecosystems by the urban atmosphere.