Non-optimal early childhood development adversely affects educational attainment, productivity, and income, and may result in inter-generational cycles of non-optimal development and poverty. Optimal development requires multiple inputs including a stimulating environment and responsive care. Given the interest in being able to monitor, at a global level, children’s exposure to positive and stimulating home environments, this paper aims to evaluate the suitability of the Family Care Indicators for this purpose. We review existing research about the features of home environments that are most important for supporting optimal early childhood development and how these features have been measured, with attention to the Family Care Indicators that have several distinct advantages for global monitoring. We report on several analyses using data from multi-country Multiple Indicator Cluster Surveys that address the validity and international comparability of the Family Care Indicators. We conducted these analyses using correlations and item response theory models to examine validity and cross-country equivalence. Based on prior studies that established validity of Family Care Indicators and on analyses reported in this paper, the items on early stimulation and responsive care from the set of Family Care Indicators will provide a valid and cross-country equivalent measure to monitor the percentage of young children experiencing positive and stimulating home environments. Additional work examining relationships between the Family Care Indicators and child development measures would further establish predictive validity.