To our knowledge, this is the first study to characterize the organization and development of large-scale human brain networks in children. We used graph-theoretical metrics to measure and characterize global and local functional brain organization in children and young-adults. The main findings of our study are: (1) large-scale brain networks in 7–9-y-old children showed similar small-world, nonrandom, functional organization at the global level, as young-adults; (2) compared to young-adults, functional brain networks in children showed significantly lower levels of hierarchical organization; (3) children and young-adults had significantly different interregional connectivity patterns, more specifically stronger subcortical-cortical and weaker cortico-cortical connectivity in children; and (4) the development of large-scale brain connectivity involves functional segregation and integration, characterized by a shift from stronger short-range connections in children to stronger long-range connections in young-adults. Collectively, these and other findings reported here provide new insights into the development of large-scale brain organization in children.