Regular physical activity and limiting extended periods of sitting are two behaviours critical for the prevention of obesity in young people. The purpose of the systematic review was to synthesize the psychometric evidence for self-report use-of-time tools that assess these behaviours. Articles were retrieved that reported reliability and/or validity for use-of-time tools in participants aged 18 years or under. Outcome variables were physical activity, sedentary behaviour and energy expenditure. Study quality was appraised, and the results summarized narratively. Sixteen studies and six different tools were identified. The tools were the Previous Day Physical Activity Recall, the Three-Day Physical Activity Recall, the Physical Activity Interview, the Computerized Activity Recall, the Activitygram, and the Multimedia Activity Recall for Children and Adolescents. Overall, tools indicated moderate validity compared with objective and criterion comparison methods. Generally, validity correlation coefficients were in the range of 0.30–0.40. Correlation coefficients for test–retest reliability ranged widely from 0.24 to 0.98. Conclusion: Use-of-time tools have indicated moderate reliability and validity for the assessment of physical activity and energy expenditure. Future research should focus on using criterion methods and on validating specifically for sedentary behaviour outcomes. Implementation of these tools for population surveillance should be considered.