Sedentary time (too much sitting) increasingly is being recognized as a distinct health risk behavior. This paper reviews the reliability and validity of self-reported and device-based sedentary time measures and provides recommendations for their use in population-based studies. The focus is on instruments that have been used in free-living, population-based research in adults. Data from the 2003–2006 National Health and Nutrition Examination Survey are utilized to compare the descriptive epidemiology of sedentary time that arises from the use of different sedentary time measures. A key recommendation from this review is that, wherever possible, population-based monitoring of sedentary time should incorporate both self-reported measures (to capture important domain- and behavior-specific sedentary time information) and device-based measures (to measure both total sedentary time and patterns of sedentary time accumulation).