Technology-based methods for assessing diet in those with disability remains largely unexplored. The aim was to assess the feasibility of assessing diet with an image-based mobile food record application (mFR) in 51 adolescents and young adults with Down syndrome (PANDs). Adherence was also assessed with the instruction to include a fiducial marker object in the before and after eating images. The PANDs sample completed a four-day mFR and results were compared with a sample of young adults from the Connecting Health and Technology study (CHAT, n = 244). Compared to the CHAT sample, PANDs participants reported more fruit (2.2 ± 1.8 versus 1.0 ± 0.9 serves respectively) and vegetables (2.4 ± 1.3 versus 1.9 ± 1.0 serves, respectively), but no differences in energy-dense nutrient-poor (EDNP) foods and beverages were observed. Compared to CHAT, PANDs participants captured fewer images with the mFR (4.9 ± 2.3 versus 4.0 ± 1.5 images, respectively). Adherence to the instruction to include the fiducial marker in images was lower for PANDs compared with the CHAT sample (90.3% versus 96.5%). Due to the quality of information captured in images and the high acceptability of the fiducial marker, the mFR shows great promise as a feasible method of assessing diet in adolescents and young adults with Down syndrome.