This longitudinal study examined associations between three after-school program quality features (positive staff-child relations, available activities, programming flexibility) and child developmental outcomes (reading and math grades, work habits, and social skills with peers) in Grade 2 and then Grade 3. Participants (n = 120 in Grade 2, n = 91 in Grade 3) attended after-school programs more than 4 days per week, on average. Controlling for child and family background factors and children's prior functioning on the developmental outcomes, positive staff-child relations in the programs were positively associated with children's reading grades in both Grades 2 and 3, and math grades in Grade 2. Positive staff-child relations also were positively associated with social skills in Grade 2, for boys only. The availability of a diverse array of age-appropriate activities at the programs was positively associated with children's math grades and classroom work habits in Grade 3. Programming flexibility (child choice of activities) was not associated with child outcomes. © 2010 The Author(s).