Background:Limited evidence links air pollution exposure to chronic cough and sputum production. Few reports have investigated the association between long-term exposure to air pollution and classically defined chronic bronchitis.Objectives:Our objective was to estimate the association between long-term exposure to particulate matter (diameter , ; , ), nitrogen dioxide , and both incident and prevalent chronic bronchitis.Methods:We estimated annual average , , and concentrations using a national land-use regression model with spatial smoothing at home addresses of participants in a prospective nationwide U.S. cohort study of sisters of women with breast cancer. Incident chronic bronchitis and prevalent chronic bronchitis, cough and phlegm, were assessed by questionnaires.Results:Among 47,357 individuals with complete data, 1,383 had prevalent chronic bronchitis at baseline, and 647 incident cases occurred over 5.7-y average follow-up. No associations with incident chronic bronchitis were observed. Prevalent chronic bronchitis was associated with [adjusted odds ratio (aOR) per interquartile range (IQR) difference ; 95% confidence interval (CI): 1.01, 1.13]. In never-smokers, was associated with prevalent chronic bronchitis ( per IQR difference; 95% CI: 1.04, 1.34), and was associated with prevalent chronic bronchitis (; ), cough (; 95% CI: 1.05, 1.16), and phlegm (; 95% CI: 1.01, 1.14); interaction p-values (nonsmokers vs. smokers) .Conclusions: exposure was related to chronic bronchitis prevalence. Among never-smokers, and exposure was associated with chronic bronchitis and component symptoms. Results may have policy ramifications for regulation by providing evidence for respiratory health effects related to long-term exposure. https://doi.org/10.1289/EHP2199