Measures that capture diet as validly and reliably as possible are cornerstones of nutritional research, and mobile-based devices offer new opportunities to improve and simplify data collection. The balance between precision and acceptability of these data collection tools remains debated, and rigorous validations are warranted. Our objective was to develop and evaluate an electronic mobile-based food record for a research setting. We developed e-CA, which includes almost 900 foods and beverages classified in 14 categories and 60 subcategories. e-CA was evaluated using three different methods: (1) usability and acceptability through a logbook and qualitative interviews; (2) dietary intake accuracy through comparison with 2 unannounced 24-h phone recalls on overlapping days; and (3) reliability and process comparison with a paper-based food record in a laboratory setting with a randomized design. e-CA proved to be intuitive and practical and was perceived as modern, trendy, and fun. Comparisons of e-CA with 24-h telephone recalls or paper-based food records in a laboratory setting with two small convenient samples showed good agreement but highlighted the well-known difficulty of estimating portion sizes and a necessary learning time to use the app. e-CA is a functional tool that has the potential to facilitate food intake measurement for research by increasing the pleasure of using the food record tool and reducing the perceived burden for the participants. It also decreases the workload, costs and the risk of transcription errors for researchers.