This study examines the quality of infant center care in Portugal through a multi-measure approach and investigates the associations among process quality dimensions and structural quality indicators. Ninety infant child care classrooms were observed during two full mornings with the Infant/Toddler Environment Rating Scale (ITERS-R), the Classroom Assessment Scoring System-Infant (CLASS-Infant) and the Caregiver Interaction Scale (CIS). Results revealed that a two-factor structure of process quality with the domains (a) Relationships and (b) Use of Space and Materials provided the best fit to the data. Of the structural indicators that were examined, teacher training showed the most robust relation to both process quality domains. In addition, classrooms with smaller groups and in centers located in non-urban areas were likely to show more sensitive relationships between teachers and infants. These findings have implications for public policy and professional development efforts on infant center care. (author abstract)