Research linking high-quality child care programs and children's cognitive development has contributed to the growing popularity of child care quality benchmarking efforts such as quality rating and improvement systems (QRIS). Consequently, there has been an increased interest in and a need for approaches to identifying thresholds, or cutpoints, in the child care quality measures used in these benchmarking efforts that differentiate between different levels of children's cognitive functioning. To date, research has provided little guidance to policymakers as to where these thresholds should be set. Using the Early Childhood Longitudinal Study, Birth Cohort (ECLS-B) data set, this study explores the use of generalized additive modeling (GAM) as a method of identifying thresholds on the Infant/Toddler Environment Rating Scale (ITERS) in relation to toddlers' performance on the Mental Development subscale of the Bayley Scales of Infant Development (the Bayley Mental Development Scale Short Form–Research Edition, or BMDSF-R). The present findings suggest that simple linear models do not always correctly depict the relationships between ITERS scores and BMDSF-R scores and that GAM-derived thresholds were more effective at differentiating among children's performance levels on the BMDSF-R. Additionally, the present findings suggest that there is a minimum threshold on the ITERS that must be exceeded before significant improvements in children's cognitive development can be expected. There may also be a ceiling threshold on the ITERS, such that beyond a certain level, only marginal increases in children's BMDSF-R scores are observed.