Background: This study investigates the association between self-rated health and the time spent in sedentary behavior (SB), low light-intensity physical activity (LLPA), high light-intensity physical activity (HLPA), and moderate to vigorous physical activity (MVPA), by controlling for demographics, socioeconomic status, and chronic diseases. Methods: A total of 1665 participants (55% women) completed a questionnaire about demographics, chronic diseases, and anthropometric characteristics and provided objective physical activity data on time in SB, LLPA, HLPA, and MVPA, using an ActiGraph 7164 accelerometer. Association between self-rated health and activity data was explored in a compositional data analysis. Results: The multinomial logistic regression analysis showed a significantly lower time spent in MVPA in proportion to time in other movement behaviors (SB, LLPA, and HLPA) for participants who rated their health as alright or poor compared with excellent (P < .001). Participants with poor, compared with excellent health, spent about a third of the time in MVPA (17 vs 50 min), marginally higher time in HLPA (134 vs 125 min), more time in LLPA (324 vs 300 min), and similar time in SB (383 vs 383 min), accounting for confounders and time in other movement behaviors. Conclusions: Promoting MVPA, as opposed to time in other movement behaviors, is suggested to be beneficial for excellent self-rated health.