Background: Wrist-worn accelerometry is the commonest objective method for measuring physical activity in large-scale epidemiological studies. Research-grade devices capture raw triaxial acceleration which, in addition to quantifying movement, facilitates assessment of orientation relative to gravity. No population-based study has yet described the interrelationship and variation of these features by time and personal characteristics. Methods: 2,043 United Kingdom adults (35–65 years) wore an accelerometer on the non-dominant wrist and a chest-mounted combined heart-rate-and-movement sensor for 7 days free-living. From raw (60 Hz) wrist acceleration, we derived movement (non-gravity acceleration) and pitch and roll (forearm) angles relative to gravity. We inferred physical activity energy expenditure (PAEE) from combined sensing and sedentary time from approximate horizontal arm angle coupled with low movement. Results: Movement differences by time-of-day and day-of-week were associated with forearm angles; more movement in downward forearm positions. Mean (SD) movement was similar between sexes ∼31 (42) mg, despite higher PAEE in men. Women spent longer with the forearm pitched >0°, above horizontal (53% vs 36%), and less time at <0° (37% vs 53%). Diurnal pitch was 2.5–5° above and 0–7.5°below horizontal during night and daytime, respectively; corresponding roll angles were ∼0° (hand flat) and ∼20° (thumb-up). Differences were more pronounced in younger participants. All diurnal profiles indicated later wake-times on weekends. Daytime pitch was closer to horizontal on weekdays; roll was similar. Sedentary time was higher (17 vs 15 hours/day) in obese vs normal-weight individuals. Conclusions: More movement occurred in forearm positions below horizontal, commensurate with activities including walking. Findings suggest time-specific population differences in behaviors by age, sex, and BMI.