Food choices are shifting globally in ways that are negatively affecting both human health and the environment. Here we consider how consuming an additional serving per day of each of 15 foods is associated with 5 health outcomes in adults and 5 aspects of agriculturally driven environmental degradation. We find that while there is substantial variation in the health outcomes of different foods, foods associated with a larger reduction in disease risk for one health outcome are often associated with larger reductions in disease risk for other health outcomes. Likewise, foods with lower impacts on one metric of environmental harm tend to have lower impacts on others. Additionally, of the foods associated with improved health (whole grain cereals, fruits, vegetables, legumes, nuts, olive oil, and fish), all except fish have among the lowest environmental impacts, and fish has markedly lower impacts than red meats and processed meats. Foods associated with the largest negative environmental impacts—unprocessed and processed red meat—are consistently associated with the largest increases in disease risk. Thus, dietary transitions toward greater consumption of healthier foods would generally improve environmental sustainability, although processed foods high in sugars harm health but can have relatively low environmental impacts. These findings could help consumers, policy makers, and food companies to better understand the multiple health and environmental implications of food choices.