This study evaluated the daily, temporal associations between sleep and daytime physical activity and sedentary behavior among adolescents from the Fragile Families & Child Wellbeing Study. A sub-sample of the cohort at age 15 (N = 417) wore actigraphy monitors for one week during the school year from which we derived daily minutes in sedentary and moderate-to-vigorous physical activity (MVPA) and nighttime sleep measures. Multilevel models tested temporal associations of nightly sleep onset, offset, duration, and sleep maintenance efficiency, with daily MVPA and sedentary behavior. More MVPA than an individual's average was associated with earlier sleep onset (p < 0.0001), longer duration (p = 0.03), and higher sleep maintenance efficiency (p < 0.0001). On days with more sedentary behavior than an individual's average, sleep onset and offset were delayed (p < 0.0001), duration was shorter (p < 0.0001), and sleep maintenance efficiency was higher (p = 0.0005). Conversely, nights with earlier sleep onset predicted more next-day sedentary behavior (p < 0.0001), and nights with later sleep offset and longer sleep duration were associated with less MVPA (p < 0.0001) and less sedentary time (p < 0.0001, p = 0.004) the next day. These bidirectional associations between sleep and physical activity suggest that promoting MVPA may help to elicit earlier bedtimes, lengthen sleep duration, and increase sleep efficiency, critical for healthy adolescent development.