Reflection spectroscopy is an emerging approach for noninvasively assessing dermal carotenoids as a biomarker of fruit and vegetable (FV) intake. This study sought to profile and identify determinants of scores from a reflection spectroscopy device (the Veggie Meter (VM)®) among 297 urban, primarily Hispanic low-income adults served by the Special Supplemental Nutrition Program for Women, Infants, and Children (WIC). The repeatability of the scores and bi- and multivariate relationships between VM scores, self-reported FV intake measured by a brief screener, and participant characteristics were examined. The mean VM score was 270 (range 0–695); 3- and 6-month test-retest correlations were positive and strong (r = 0.79 and 0.55, respectively). VM scores were negatively associated with body mass index (BMI; r = −0.22) and were higher among participants of Ecuadorian, Dominican, and Mexican Hispanic origin relative to those of Puerto Rican origin; foreign- vs. US-born participants, breastfeeding vs. non-breastfeeding participants, nonsmokers vs. smokers, and participants who consumed three or more cups of FV/day relative to those who consumed less than three cups of FV/day. Foreign-born nativity, consumption of three or more cups of FV/day, and smaller body size were determinants of increased VM scores. Although replication studies are needed to confirm these findings, investigators working with similar populations are encouraged to use the VM to longitudinally track FV intake and to target determinants of the scores in observational and intervention studies of FV intake as measured by the VM.