Although many youths participate in afterschool programs, the research is unclear about which aspects of afterschool program quality contribute most to positive outcomes. This article examines the relationship among quality and outcomes of 21st Century Community Learning Centers (CLCCs) afterschool programs, as perceived by 3,388 stakeholders from 337 21st CLCCs in one midwestern state. Perceptions were gathered using the Ohio Quality Assessment Rubric. Descriptive frequencies were generated to identify cross-site strengths and weaknesses, and a canonical correlation was conducted to identify which quality indicators were most related to perceived outcomes. Stakeholders perceived quality across multiple program areas, but the indicator most strongly correlated to outcomes was that of family engagement strategies, an area of relatively poor performance among participating sites. Perceptions of the quality of general youth development strategies and of facilities, space, and equipment were the most favorable among stakeholders. These factors held the weakest correlations with outcomes. These patterns have implications for 21st CLCCs, schools, afterschool partners, and school social workers looking to improve the quality of programs to achieve better youth outcomes.