In the context of continuing ecosystem degradation and deepening socio-economic inequality, sustainability scientists must question the adequacy of current scholarship and practice. We argue that pre-occupation with external phenomena and collective social structures has led to the neglect of people’s ‘inner worlds’—their emotions, thoughts, identities and beliefs. These lie at the heart of actions for sustainability, and have powerful transformative capacity for system change. The condition of people’s inner worlds ought to also be considered a dimension of sustainability itself. Compassion, empathy and generosity, for example, are personal characteristics that mark individual expressions of sustainability. Sustainability science must take inner life more seriously by considering how language shapes and is shaped by paradigms about the world, prioritising enquiry into how spirituality, contemplation and sustainability transformation relate, and encouraging scholars and practitioners to intentionally cultivate their inner worlds to strengthen inner resources necessary for addressing sustainability challenges.