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(1) Background: Smartphone dietary assessment apps can be acceptable and valid data collection methods but have predominantly been validated in highly educated women, and none specifically measured eating-out habits in young adults. (2) Methods: Participants recorded their food and beverage consumption for three days using the Eat and Track (EaT) app, and intakes were compared with three dietitian-administered 24-h recall interviews matched to the same days as the reference method. Wilcoxon signed-rank or t-tests, correlation coefficients and Bland–Altman plots assessed agreement between the two methods for energy and percentage energy from nutrients (%E). (3) Results: One hundred and eighty nine of 216 participants (54% females, 60% resided in higher socioeconomic areas, 49% university-educated) completed the study. There were significant differences in median energy intake between methods (p < 0.001), but the EaT app had acceptable agreement for most nutrient densities at the group level. Correlation coefficients ranged from r = 0.56 (%E fat) to 0.82 (%E sugars), and between 85% and 94% of participants were cross-classified into the same or adjacent quartiles. Bland–Altman plots showed wide limits of agreement but no obvious biases for nutrient densities except carbohydrate in males. (4) Conclusions: The EaT app can be used to assess group nutrient densities in a general population of 18-to-30-year olds.

Technology-enhanced methods of dietary assessment may still face common limitations of self-report. This study aimed to assess foods and beverages omitted when both a 24 h recall and a smartphone app were used to assess dietary intake compared with camera images. For three consecutive days, young adults (18–30 years) wore an Autographer camera that took point-of-view images every 30 seconds. Over the same period, participants reported their diet in the app and completed daily 24 h recalls. Camera images were reviewed for food and beverages, then matched to the items reported in the 24 h recall and app. ANOVA (with post hoc analysis using Tukey Honest Significant Difference) and paired t-test were conducted. Discretionary snacks were frequently omitted by both methods (p < 0.001). Water was omitted more frequently in the app than in the camera images (p < 0.001) and 24 h recall (p < 0.001). Dairy and alternatives (p = 0.001), sugar-based products (p = 0.007), savoury sauces and condiments (p < 0.001), fats and oils (p < 0.001) and alcohol (p = 0.002) were more frequently omitted in the app than in the 24 h recall. The use of traditional self-report methods of assessing diet remains problematic even with the addition of technology and finding new objective methods that are not intrusive and are of low burden to participants remains a challenge.