Background: State afterschool networks across the US are engaged in system-building efforts to improve the quality of science, technology, engineering, and math (STEM)-focused afterschool programming. This study examined national trends in STEM program quality, youth outcomes, and the connections between these two data sources. Methods: One thousand five hundred ninety-nine youths (grades 4-12) enrolled in 158 STEM-focused afterschool programs across 11 state networks completed a retrospective self-assessment measuring STEM attitudes and socialemotional learning (SEL)/twenty-first-century skills. Two hundred fifty standardized observations of STEM activities were performed to measure STEM program quality. Results: (1) Most youth (65-85%) reported increases in STEM engagement, identity, career interest, career knowledge, relationships, critical thinking, and perseverance, with the largest gains reported by those engaging with STEM activities for 4 weeks or more; (2) there were significant, strong correlations between STEM and SEL/twenty-first-century outcomes reported by youth; and (3) youth participating in higher-quality STEM programming reported more growth than peers participating in lower-quality programs. Conclusion: This effort demonstrates how investments in STEM program quality yield high returns for programs and youth and how collaborations between research and practice can track successes and challenges, determine investments in program management, and expand advocacy and policy efforts. Additionally, this study supports a growing body of literature that suggests a synergy between youth development and STEM learning approaches that can improve outcomes for youth.