The purpose of this study was to test the utility of the Toddler CARE-Index, an assessment tool for parent-child interaction among preschool-aged children, for screening of parental sensitivity. The CARE-Index was initially developed for infants and had been adapted for toddlers up to 3 years of age. This study tests its utility for children up to 5.8 years old. Sixty-four children (2.3 to 5.8 years) and their mothers took part in the study and were examined with both the Toddler CARE-Index and the Preschool Assessment of Attachment. The sample comprised two groups, a sample that had come to professional attention (n = 21) and a normative sample (n = 43). Analysis of coder agreement showed adequate correspondence among three coders. Test-retest reliability was less robust. Testing validity, there was a significant relation between sensitivity of the mother and attachment security of the child in the total sample as well as in both subsamples. These results are a first step for using the Toddler CARE-Index as an economical and promising instrument for the assessment of parental sensitivity with children beyond toddlerhood in both normative and clinical settings.