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Recent years have witnessed a steady growth of time-use research, driven by the increased research and policy interest in population activity patterns and their associations with long-term outcomes. There is recent interest in moving beyond traditional paper-administered time diaries to use new technologies for data collection in order to reduce respondent burden and administration costs, and to improve data quality. This paper presents two novel diary instruments that were employed by a large-scale multi-disciplinary cohort study in order to obtain information on the time allocation of adolescents in the United Kingdom. A web-administered diary and a smartphone app were created, and a mixed-mode data collection approach was followed: cohort members were asked to choose between these two modes, and those who were unable or refused to use the web/app modes were offered a paper diary. Using data from a pilot survey of 86 participants, we examine diary data quality indicators across the three modes. Results suggest that the web and app modes yield an overall better time diary data quality than the paper mode, with a higher proportion of diaries with complete activity and contextual information. Results also show that the web and app modes yield a comparable number of activity episodes to the paper mode. These results suggest that the use of new technologies can improve diary data quality. Future research using larger samples should systematically investigate selection and measurement effects in mixed-mode time-use survey designs.