Philanthropic organizations are experimenting with ways to support capacity building in order to scale innovations and leverage funding for greater social impact. Increasingly, philanthropies are also attending to their own organizational needs for learning in order to inform strategy, shape future work, and measure effectiveness. This article shares the lessons of the Aligned Partners Project, a three-year study of a foundation-funded interorganizational collaboration to align the work of three technical assistance organizations to meet the needs of one school district. It identifies challenges to providing coherent assistance as well as grantmaking practices that could address them. A foundation seeking to fund an education-improvement project is encouraged to work with all key stakeholders in the earliest stages to establish a learning agenda, hire a partner outside the project to facilitate that agenda's development, and involve district stakeholders in project goals and design. This article also argues for awarding research grants as a capacity-building strategy to support grantees and grantmaking organizations, and to yield greater impact in the field.