Cross-sector cradle-to-career initiatives are increasingly central to communities' strategies to support children and youth. StriveTogether Cradle to Career Civic Infrastructure provides a framework for how a community comes together around a vision; improves and builds upon those efforts over time; and invests the community's resources differently to increase impact. This brief uses lessons learned from The After-School Corporation's (TASC), ExpandED Schools, a national effort that aligns youth-serving community organizations and schools to add approximately three hours of learning time to the conventional school day, to describe the role of non-profit organizations in the StriveTogether Framework, and to provide recommendations for expanding and enhancing their role in achieving collective impact.