Background: Carbohydrate-rich (CR) foods are essential parts of the Chinese diet. However, CR foods are often given less attention than animal-based foods. The objectives of this study were to analyze the carbon emissions caused by CR foods and to generate sustainable diets with low climate impact and adequate nutrients. Methods: Twelve common CR food consumption records from 4857 individuals were analyzed using K-means clustering algorithms. Furthermore, linear programming was used to generate optimized diets. Results: Total carbon emissions by CR foods was 683.38g CO₂eq per day per capita, accounting for an annual total of 341.9Mt CO₂eq. All individuals were ultimately divided into eight clusters, and none of the popular clusters were low carbon or nutrient sufficient. Optimized diets could reduce about 40% of carbon emissions compared to the average current diet. However, significant structural differences exist between the current diet and optimized diets. Conclusions: To reduce carbon emissions from the food chain, CR foods should be a research focus. Current Chinese diets need a big change to achieve positive environmental and health goals. The reduction of rice and wheat-based foods and an increase of bean foods were the focus of structural dietary change in CR food consumption.