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The effects of center-based care on early development, outside of carefully controlled demonstration programs, appear to be positive yet often modest for children from low-income families. But little is known about variation in the quality of centers and preschools found among low-income neighborhoods. Evidence also remains scarce on the observed quality of home-based care, the settings that most children attend and into which large infusions of federal dollars are now directed. This paper reports on the observed quality of 166 centers and 187 nonparental home settings (including family child care homes and kith or kin providers) serving children in five cities situated in California, Connecticut, or Florida. Centers displayed higher mean quality as gauged by provider education and the intensity of structured learning activities, compared to home-based settings, but did not consistently display more positive child–provider interactions. Great variability among centers and home-based settings was observed, including between-city differences. Second, we found that contextual neighborhood attributes accounted for the quality of providers selected more strongly than family-level selection factors. Mothers with stronger verbal abilities (PPVT scores) did select higher quality centers; those employed longer hours each week relied on kith and kin providers with lower education levels. Interrelationships among different quality measures are detailed. The policy implications of such wide disparities in center and home-based care quality are discussed, including how states could more carefully strengthen regulatory or quality improvement efforts.