To advance the field of time-use epidemiology, a tool capable of monitoring 24 h movement behaviours including sleep, physical activity, and sedentary behaviour is needed. This study explores compliance with a novel dual-accelerometer system for capturing 24 h movement patterns in two free-living samples of children and adults. A total of 103 children aged 8 years and 83 adults aged 20-60 years were recruited. Using a combination of medical dressing and purpose-built foam pouches, participants were fitted with two Axivity AX3 accelerometers—one to the thigh and the other to the lower back—for seven 24 h periods. AX3 accelerometers contain an inbuilt skin temperature sensor that facilitates wear time estimation. The median (IQR) wear time in children was 160 (67) h and 165 (79) h (out of a maximum of 168 h) for back and thigh placement, respectively. Wear time was significantly higher and less variable in adults, with a median (IQR) for back and thigh placement of 168 (1) and 168 (0) h. A greater proportion of adults (71.6%) achieved the maximum number of complete days when compared to children (41.7%). We conclude that a dual-accelerometer protocol using skin attachment methods holds considerable promise for monitoring 24-h movement behaviours in both children and adults.