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The facilitation of Education for Sustainability (EfS) by Decentralized Global Networks (DGNs) is consistent with the dynamic and increasingly complex nature of sustainability issues, and is often motivated by inter-governmental policy objectives that link sustainability learning with sustainable development. The use of DGNs for EfS is now well established and supports the participation of a geographically dispersed and diverse body of participants that consist of teachers, teacher-educators, policy makers, and researchers. However, there is limited understanding of the complex systems operating within DGNs and how these systems generate the conditions necessary to facilitate EfS. In this article, the authors report on an interpretive case study of the Environment and Schools Initiative (ENSI), a DGN operating for over 26 years with a membership that has spanned over 25 countries. Findings highlight six dimensions of the ENSI DGN important to the effective facilitation of EfS including: (1) developing a community of practice; (2) planning for phased organizational development; (3) structured decentralization using a strategy-node-program framework; (4) linking research to practice; (5) ensuring relevance through contextualized approaches; and (6) monitoring and evaluation of processes and outcomes. The findings identify organizational level approaches to EfS facilitation such as addressing the nexus created between policy, practice and research, and developing a structure focused on learning and the development of networks more broadly. In conclusion, the delivery of learning and teaching strategies through a geographically dispersed and diverse group of participants can address the inherent complexity of EfS facilitation across various spatial and cultural scales. Full article