Drawing on Coleman’s concept of social capital, researchers have investigated how the quality of neighborhood social networks influences child development and well-being. The role of non-kin older neighbors in advancing child well-being through the enhancement of social capital, however, has been under-studied. Our objective was to delineate specific pathways through which non-kin older neighbors contribute to neighborhood quality for children and families and potentially advance child well-being. We examined open-ended interview data from 400 parents who cared for at least one child under 18 years of age and resided in 20 neighborhoods in Cleveland, Ohio. A subsample of 113 parents connected older neighbors to neighborhood quality for families and children in their narratives. Our analysis identified three primary pathways through which parents positively linked older neighbors to neighborhood quality: older neighbors support parents and children, promote neighborhood safety, and contribute to neighborhood residential stability. These contributions are evidence of intergenerational closure, reciprocated exchange, and informal social control working together to create social capital in neighborhoods for children. It is by enhancing social capital that older neighbors potentially improve child well-being. We discuss the implications of our findings for neighborhood research and practice.