Quality learning for sustainability can have a transformative effect in terms of promoting empowerment, leadership and wise investments in individual and collective lives and regenerating the local economies of cities, making them more inclusive, safe, resilient and sustainable. It can also help cities move towards achieving the United Nations Sustainable Development Goals (SDGs). Effecting the transformation of cities into Learning Cities, however, requires changes in the structure of governance. Drawing on interviews with key informants as well as secondary data, this article examines how collaborative governance has facilitated quality learning for sustainability in Bristol (United Kingdom), Kitakyushu (Japan) and Tongyeong (Republic of Korea). Focusing on a conceptual framework and practical application of learning initiatives, this comparative study reveals how these cities' governance mechanisms and institutional structures supported initiatives premised on cooperative learning relationships. While recognising differences in the scope and depth of the learning initiatives and the need for further improvements, the authors found evidence of general support for the governance structures and mechanisms for learning in these cities. The authors conclude by recommending that (1) to implement the Learning Cities concept based on UNESCO's "Key Features of Learning Cities", recognition should be given to existing sustainability-related learning initiatives in cities; (2) collaborative governance of the Learning Cities concept at both local and international levels should be streamlined; and (3) UNESCO's Global Network of Learning Cities could serve as a hub for sharing education/learning resources and experiences for other international city-related programmes as an important contribution to the implementation of the SDGs.