This study investigated the association between the allocation of time-use over the 24-h day between sleep, sedentary behaviour (SB), light-intensity physical activity (LPA) and moderate-to-vigorous-intensity physical activity (MVPA)) and health indicators. A cross-sectional analysis of Canadian Health Measures Survey data was undertaken using compositional data analysis. SB, LPA and MVPA were derived from Actical accelerometers, whilst sleep was self-reported by respondents. The analysis was stratified by age; adults (aged 18–64 years; n = 6322) and older adults (65–79 years; n = 1454). For adults, beneficial associations were observed between larger proportions of MVPA relative to time in other behaviours and body mass index (BMI), waist circumference, aerobic fitness, resting heart rate, high-density lipoprotein (HDL) cholesterol, triglycerides, blood glucose and insulin levels. More time spent in sleep relative to other movement behaviours was deleteriously associated with aerobic fitness, HDL cholesterol, insulin, C-reactive proteins and grip strength but beneficially with low-density lipoprotein cholesterol. Relative time spent in LPA was deleteriously associated with BMI and beneficially with triglycerides and grip strength. In older adults, these associations were blunted or disappeared but larger proportions of MVPA were associated with better mental health. The importance to health of MVPA when explicitly considered relative to other movement behaviours was confirmed.