Commonly regulated structural quality features, like educator education levels and group size, are thought to be foundational to the quality of children’s everyday experiences in early education and care settings. Yet little is known about how these features relate to the day-to-day interactions and activities that occur in these settings—or process quality features—across the landscape of early education and care. In this study, we examine the association between structural quality features and process quality features in a diverse sample of classrooms (n = 672) participating in a statewide study of early education and care. Using a permutation test approach, we found that group size and child-to-adult ratio were most consistently linked to children’s experiences but educator education, experience, and curriculum usage were largely unrelated. Implications of these findings for quality improvement initiatives are discussed. (author abstract)