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Daily interactions build children’s self-regulation but studying self-regulation at the daily level is challenging. This study examined the validity of wearable accelerometers to index daily variability in aspects of children’s behavioral regulation. Using data from the Study of Early Child Care and Youth Development (N = 1,364, 51% male, 81% Non-Hispanic White), accelerometers captured the number of times children initiated movement at school in third grade, showing concurrent validity with teacher reports of behavioral regulation most closely related to motor activity, modest correlations with teacher reports of related skills like attention and social self-control, but low associations with assessments of cognitive regulation. Latent growth modeling revealed downward trajectories in accelerometer-assessed behavior and teacher reports of hyperactivity/impulsivity from third grade to sixth grade and associations across measures between children’s initial levels, rintercepts = .44, p < .001, and rates of decline, rslopes = .42, p = .003. Children’s accelerometer-assessed behavior in third grade predicted age 15 impulsivity, β = 0.15, p = .002, academic achievement, β = -0.13, p = .003, and risk-taking, β = 0.10, p = .017. Examining accelerometer-assessed behavior across days in third grade (N = 4,051), half of the variance was within-child, ICC = .47. An exploratory within-child analysis revealed more dysregulated behavior on Fridays, β = .16, p < .001. Wearable accelerometers can detect changes in children’s behavioral regulation across days, enabling studies at the daily level.