Food insecurity and the nutrition transition have been noted in arctic communities. We therefore evaluated biomarkers of nutritional status and nutrient intakes by traditional food (TF) and food security status among Inuit in Canada. A cross-sectional health survey of Inuit (≥18 y) in 36 arctic communities was conducted in 2007-2008. Food security was assessed by 24-h dietary recalls using USDA questionnaires and nutrient intakes. Biomarkers included serum 25-hydroxy vitamin D [25(OH)D], hemoglobin, serum ferritin, and erythrocyte RBC fatty acids (FA). Analyses were stratified by past-day TF consumption (yes vs. no) and food security status (secure vs. insecure). Food insecurity was prevalent (62.6%) and associated with higher RBC trans-FA and lower hemoglobin levels and serum ferritin, whereas TF consumption was associated with higher serum 25(OH)D, (n-3) FA, and serum ferritin (P ≤ 0.05). In men, food insecurity was associated with lower intake of energy and energy-adjusted fiber, vitamin C, iron, zinc, and magnesium. In women, food insecurity was associated with a higher intake of carbohydrates and lower intake of fiber, dietary folate equivalent, vitamin C, iron, magnesium, calcium, and vitamin D. For both sexes, when TF was consumed, there was a higher intake of protein, protein-related micronutrients, and vitamins A and C and a lower intake of carbohydrates, saturated fat, and fiber and a lower sodium:potassium ratio (P ≤ 0.05). Nutrition transition and food insecurity are associated with a multifaceted shift in nutrient status and intakes with implications for increased risk of diet-sensitive chronic diseases.