This study aimed to investigate differences in physical activity (PA) patterns and the associations between objectively measured 24-h movement behaviors and musculoskeletal measures (muscle strength, muscle mass, physical performance, and bone mineral density) in a high-income and a low-income community. This cross-sectional study recruited independent living older adults aged 60–85 years from high-income Scottish (n = 150) and low-income South African (n = 138) settings. Participants completed demographic and health questionnaires, and testing included body composition and bone mineral density (dual energy X-ray absorptiometry), physical performance (grip strength, gait speed), and PA (accelerometry). Participants accumulated similar amounts of weekly total PA, however, the Scottish cohort engaged in more moderate-to-vigorous intensity PA (MVPA) and sedentary behavior (SB), while the South African cohort spent more time sleeping and in light intensity PA (LPA). From compositional data analysis, more time spent in MVPA relative to the other movement behaviors was positively associated with higher muscle mass (p < 0.001) and strength (p = 0.001) in the Scottish cohort. Conversely, more time spent in MVPA was associated with faster gait speed (p < 0.001) and greater hip bone mineral density (p = 0.011) in the South African cohort. Our findings confirm the beneficial role of MVPA in both high- and low-income cohorts, however, the relationship MVPA had with components of musculoskeletal health in older adults differed between settings.