Purpose: To describe youth time-use compositions, focusing on time spent in shorter and longer bouts of sedentary behavior and physical activity (PA), and to examine associations of these time-use compositions with cardiometabolic biomarkers. Methods: Accelerometer and cardiometabolic biomarker data from 2 Australian studies involving youths 7–13 years old were pooled (complete cases with accelerometry and adiposity marker data, n = 782). A 9-component time-use composition was formed using compositional data analysis: time in shorter and longer bouts of sedentary behavior; time in shorter and longer bouts of light-, moderate-, or vigorous-intensity PA; and “other time” (i.e., non-wear/sleep). Shorter and longer bouts of sedentary time were defined as <5 min and ≥5 min, respectively. Shorter bouts of light-, moderate-, and vigorous-intensity PA were defined as <1 min; longer bouts were defined as ≥1 min. Regression models examined associations between overall time-use composition and cardiometabolic biomarkers. Then, associations were derived between ratios of longer activity patterns relative to shorter activity patterns, and of each intensity level relative to the other intensity levels and “other time”, and cardiometabolic biomarkers. Results: Confounder-adjusted models showed that the overall time-use composition was associated with adiposity, blood pressure, lipids, and the summary score. Specifically, more time in longer bouts of light-intensity PA relative to shorter bouts of light-intensity PA was significantly associated with greater body mass index z-score (zBMI) (β = 1.79, SE = 0.68) and waist circumference (β = 18.35, SE = 4.78). When each activity intensity was considered relative to all higher intensities and “other time”, more time in light- and vigorous-intensity PA, and less time in sedentary behavior and moderate-intensity PA, were associated with lower waist circumference. Conclusion: Accumulating PA, particularly light-intensity PA, in frequent short bursts may be more beneficial for limiting adiposity compared to accumulating the same amount of PA at these intensities in longer bouts.