Background: Healthy diets are supposed to be more environmentally friendly because they rely mainly on plant-based foods, which have lower greenhouse gas emissions (GHGEs) per unit weight than do animal-based foods.Objectives: The objectives were to estimate the GHGEs associated with the consumption of self-selected diets in France and to analyze their relation with the nutritional quality of diets.Design: For each adult in the national dietary Individual and National Survey on Food Consumption (n = 1918), the GHGEs of his or her diet were estimated based on the GHGEs of 391 foods. Highest-nutritional-quality diets were defined as those having simultaneously 1) an energy density below the median, 2) a mean adequacy ratio (MAR) above the median, and 3) a mean excess ratio (MER, percentage of maximum recommended values for nutrients whose intake should be limited) below the median.Results: MAR was positively correlated and MER was negatively correlated with diet-related GHGEs. High-nutritional-quality diets contained more plant-based foods, notably fruit and vegetables, and fewer sweets and salted snacks than did low-quality diets. After adjustment for age, sex, and energy intake, the consumption of sweets and salted snacks was negatively correlated with diet-related GHGEs, whereas the consumption of animal products and of fruit and vegetables was positively associated with them. After adjustment for energy intake, high-nutritional-quality diets had significantly higher GHGEs (+9% and +22% for men and women, respectively) than did low-nutritional-quality diets.Conclusion: Despite containing large amounts of plant-based foods, self-selected diets of the highest nutritional quality are currently not those with the lowest diet-related GHGEs.