The risk of obesity during childhood can be significantly reduced through increased physical activity and decreased sedentary behavior. Recent technological advances have created opportunities for the real-time measurement of these behaviors. Mobile phones are ubiquitous and easy to use, and thus have the capacity to collect data from large numbers of people. The present study tested the feasibility, acceptability, and validity of an electronic ecological momentary assessment (EMA) protocol using electronic surveys administered on the display screen of mobile phones to assess children's physical activity and sedentary behaviors. A total of 121 children (ages 9-13, 51% male, 38% at risk for overweight/overweight) participated in EMA monitoring from Friday afternoon to Monday evening during children's nonschool time, with 3-7 surveys/day. Items assessed current activity (e.g., watching TV/movies, playing video games, active play/sports/exercising). Children simultaneously wore an Actigraph GT2M accelerometer. EMA survey responses were time-matched to total step counts and minutes of moderate-to-vigorous physical activity (MVPA) occurring in the 30 min before each EMA survey prompt. No significant differences between answered and unanswered EMA surveys were found for total steps or MVPA. Step counts and the likelihood of 5+ min of MVPA were significantly higher during EMA-reported physical activity (active play/sports/exercising) vs. sedentary behaviors (reading/computer/homework, watching TV/movies, playing video games, riding in a car) (P < 0.001). Findings generally support the acceptability and validity of a 4-day EMA protocol using mobile phones to measure physical activity and sedentary behavior in children during leisure time.