Background: Physical activity levels are low in people with chronic obstructive pulmonary disease, and there is limited knowledge about how pulmonary rehabilitation transforms movement behaviors. This study analyzed data from a pulmonary rehabilitation trial and identified determinants of movement behaviors. Methods: Objectively assessed time in daily movement behaviors (sleep, sedentary, light-intensity physical activity, and moderate- to vigorous-intensity physical activity) from a randomized controlled trial (n = 73 participants) comparing home- and center-based pulmonary rehabilitation was analyzed using conventional and compositional analytical approaches. Regression analysis was used to assess relationships between movement behaviors, participant features, and response to the interventions. Results: Compositional analysis revealed no significant differences in movement profiles between the home- and center-based groups. At end rehabilitation, conventional analyses identified positive relationships between exercise capacity (6-min walk distance), light-intensity physical activity, and moderate- to vigorous-intensity physical activity time. Compositional analyses identified positive relationships between a 6-minute walk distance and moderate- to vigorous-intensity physical activity time, accompanied by negative relationships with sleep and sedentary time (relative to other time components) and novel relationships between body mass index and light-intensity physical activity/sedentary time. Conclusion: Compositional analyses following pulmonary rehabilitation identified unique associations between movement behaviors that were not evident in conventional analyses.