Rates of atmospheric deposition are declining across the United States, yet urban areas remain hotspots of atmospheric deposition. While past studies show elevated rates of inorganic nitrogen (N) deposition in cities, less is known about atmospheric inputs of organic N, organic carbon (C), and organic and inorganic phosphorus (P), all of which can affect ecosystem processes, water quality, and air quality. Further, the effect of the tree canopy on amounts and forms of nutrients reaching urban ground surfaces is not well‐characterized. We measured growing season rates of total N, organic C, and total P in bulk atmospheric inputs, throughfall, and soil solution around the greater Boston area. We found that organic N constitutes a third of total N inputs, organic C inputs are comparable to rural inputs, and inorganic P inputs are 1.2 times higher than those in sewage effluent. Atmospheric inputs are enhanced two‐to‐eight times in late spring and are elevated beneath tree canopies, suggesting that trees augment atmospheric inputs to ground surfaces. Additionally, throughfall inputs may directly enter runoff when trees extend above impervious surfaces, as is the case with 26.1% of Boston's tree canopy. Our results indicate that the urban atmosphere is a significant source of elemental inputs that may impact urban ecosystems and efforts to improve water quality, particularly in terms of P. Further, as cities create policies encouraging tree planting to provide ecosystem services, locating trees above permeable surfaces to reduce runoff nutrient loads may be essential to managing urban biogeochemical cycling and water quality.