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Background: Adherence rates of ≥95% to antiretroviral therapy (ART) are necessary to maintain viral suppression in HIV-infected individuals. We identified predictors of nonadherence to scheduled antiretroviral drug pickup appointments in a large HIV care and treatment program in Tanzania. Methods: We performed a prospective cohort study of 44, 204 HIV-infected adults on ART between November 2004 and September 2012. Multivariate generalized estimating equation for repeated binary data was used to estimate the relative risk and 95% confidence intervals of nonadherence. Results: Nonadherence was significantly greater among patients with high CD4 counts, high body mass indices, males, younger patients, patients with longer durations on ART, and those with perceived low social support. Conclusions: Targeted interventions should be developed to improve ART adherence among healthier, younger, and more experienced patients who are on ART for longer durations within HIV care and treatment programs. Social support for patients on ART should be emphasized.