Indigenous peoples experience a disproportionate burden of food insecurity and the Arctic is no exception. We therefore evaluated the prevalence, socio-demographic, and dietary correlates of food insecurity in the most comprehensive assessment of food insecurity in Arctic Canada. A cross-sectional survey of 1901 Inuit households was conducted in 2007-2008. Measurements included food insecurity, 24-h dietary recalls, socio-demographics, and anthropometry. Food insecurity was identified in 62.6% of households (95% CI = 60.3-64.9%) with 27.2% (95% CI = 25.1-29.3%) of households severely food insecure. The percent with an elevated BMI, waist circumference, and percent body fat was lower among individuals from food insecure households compared to food secure households (P ≤ 0.001). Adults from food insecure households had a significantly lower Healthy Eating Index score and consumed fewer vegetables and fruit, grains, and dairy products, and consumed a greater percent of energy from high-sugar foods than adults from food secure households (P ≤ 0.05). Food insecurity was associated with household crowding, income support, public housing, single adult households, and having a home in need of major repairs (P ≤ 0.05). The prevalence of having an active hunter in the home was lower in food insecure compared to food secure households (P ≤ 0.05). Food insecurity prevalence is high in Inuit communities, with implications for diet quality that over the long-term would be anticipated to exacerbate the risk of diet-related chronic diseases. Actions are required to improve food security that incorporate the traditional food system and healthy market food choices.