(1) Background: Aspects of the Mongolian food supply, including high availability of animal-source foods and few plant foods, are plausibly associated with disease in the population. Data on Mongolian diets are lacking, and these risks are poorly quantified. The purpose of this study was to provide a multifaceted nutritional analysis of the modern Mongolian diet. (2) Methods: The study population consisted of 167 male and 167 female healthy non-pregnant urban and nomadic adults (22–55 years) randomly selected from lists of residents in 8 regions. From 2011–2016, 3-day weighed diet records and serum were collected twice from each participant in summer and winter; anthropometry was collected once from each participant. Serum was analyzed for biomarkers, and nutrient intake computed using purpose-built food composition data and adjusted for within-person variation. Exploratory dietary patterns were derived and analyzed for associations with diet and nutrition measurements. (3) Results: We collected 1838 of an expected 1986 diet records (92.5%), 610/658 serum samples (92.7%), and 315/334 height and weight measurements (94.3%). Sixty-one percent of men and 51% of women were overweight or obese. Consumption of red meat, refined grains, and whole-fat dairy was high, while that of fruits, non-tuberous vegetables, eggs, nuts and seeds, fish and poultry, and whole grains was low. Dairy and red meat were more consumed in summer and winter, respectively. Dietary inadequacy of 10 of 21 assessed nutrients, including fiber, folate, and vitamin D were >50% prevalent, while protein, zinc, and vitamin B12 inadequacy were low. Biochemical evidence of iron and vitamin A deficiency was also low. Three dietary patterns (Urban, Transitional, Nomadic) explained 41% of variation in food consumption. The Urban pattern was positively associated with BMI in multivariate analysis. (4) Conclusions: Results indicate a high prevalence of key dietary inadequacies and overweight among Mongolian adults. Prior studies by our group have suggested that expanded supplementation and food fortification would be effective in addressing micronutrient inadequacies; these strategies should be coupled with measures to mitigate the growing burden of chronic disease.