The steadily rising global urban population has placed substantial strain on urban water quality, and this strain is projected to increase for the foreseeable future. Considerable attention has been given to the hydrological and physico-chemical effects of urbanization on stream ecosystems. However, due to the relative infancy of the field of urban ecology, long-term water quality analyses in urban streams are sparse. Using a 15-year stream chemistry monitoring record from Baltimore, MD, USA, we quantified long-term trends in nitrate, phosphate, total nitrogen, total phosphorus, chloride, and sulfate export at several sites along a rural-urban gradient. We found no significant change in solute export at most sites, although we did find specific patterns of interest for certain solutes. For example, nitrogen export declined at the most headwater urban site, while phosphorus export declined at the most downstream urban site. Coupling long-term monitoring with data on gray and green infrastructure management throughout the landscape, we established relationships between solute export at the most downstream urban monitoring site and sanitary sewer overflows (SSOs), best management practice (BMP) implementation, and road salt application rates. Phosphorus export was correlated with BMP implementation in the watershed, whereas nitrogen export was related to SSOs. Despite highly urbanized watersheds, water quality does not appear to be declining at most of these sites, suggesting that current management may have limited further impairment. Results of our study suggest that both gray and green infrastructure are key for maintaining and improving water quality in this highly urbanized watershed.