The challenges in the characterization of the nutritional quality of grain foods comprise obstacles to public health actions toward promotion of healthier grain-based foods. The present study investigated how carbohydrate metrics related to glycemic index (GI), glycemic load (GL), and warning labels of grain foods consumed by individuals living in São Paulo, Brazil. Information on intake of grain foods at individual level was obtained using 24 h recalls within a cross-sectional population-based survey conducted in 2015. There were 244 unique grain products reported by individuals in the survey, assessed through four metrics of carbohydrate quality, considering contents per 10 g of total carbohydrate: (1) ≥1 g fiber, (2) ≥1 g fiber and p-values p-values p-value 50% of products with good nutritional quality according to the carbohydrate metrics still would receive warnings. Findings suggest that carbohydrate metrics identified products with lower GI and GL, and current warning labels may not adequately capture overall nutritional quality of grain foods.