In this cross-sectional study of 236 schoolchildren living in Manresa, Spain, we evaluated the association between prevalence of dental caries and frequency of consumption of various food groups, including sweetened baked goods and similar foods (rich in starch and sugars) and confectionery (rich in sugars but not starch), using a food-frequency questionnaire. Because Streptococcus mutans is associated with the cariogenicity of carbohydrates, we also evaluated the modification of these associations by salivary counts of this microorganism. Odds ratios (ORs) were used to measure the association between caries and tertiles of consumption. Sex, age, use of fluorides, tooth-brushing frequency, frequency of dental visits, socioeconomic status, and intake of other potentially cariogenic food groups were considered as potential confounders. We did not find a significant association between any of the food groups evaluated and caries prevalence. Failure to detect an association could have been due to the low prevalence of caries in our population (decayed, missing, or filled permanent teeth = 1.3 at age 10.6 y) or to underestimation of the association due to diet misclassification. In this population, the association between consumption of sweetened baked goods and caries appeared to be modified by the numbers of S. mutans [OR = 6.1 (95% CI: 1.6, 23.0) for low compared with high intake in children with moderate-to-high S. mutans counts and OR = 0.3 (95% CI: 0.1, 1.6) for low compared with high intake in children with low S. mutans counts]. These results suggest that a high intake of sweetened baked goods may be a determinant of caries prevalence in children with moderate-to-high salivary counts of S. mutans.