Nature-Based Solutions concepts and practices are being used worldwide as part of attempts to address societal challenges but have also been criticised for not dealing with deeper transformations needed to face urgent issues including biodiversity loss, climate change and inclusion. In this paper, we explore how an inclusive, integrated and long-sighted approach, emphasising a more radical integration of nature within cities, might support the transformations needed to endure major contemporary challenges. Addressing important emerging critiques of Nature-Based Solutions, we consider the potential of a more incisive form of Nature-Based Thinking (NBT) in cities, based on more holistic perspectives. The paper draws on a reflective and iterative research process that engaged both the research and practice communities through a symposium and a series of futures workshops that together explored the potential of NBT to develop future nature-cities relations in Europe and Latin America. The results of the reflective process suggest that notions of nature with people—not for people— new organisational structures, and the intention and capacity to apply long-term perspectives, are needed when planning for NBS interventions aimed at sustainable urban development. This includes developing a cultural-structural change based on new and inclusive understandings of human–nature relations, and novel governance paradigms that allow cross-sectoral coordination and engagement of local stakeholders beyond formal organisational structures.