Modern environmental thought has always involved normative claims about the values needed for sustainability. This has often played out in debates between proponents of anthropocentric and ecocentric ways of valuing nature. More recently, there has been a flourishing of interest in relational and pluricentric ways of valuing nature, coinciding with a “turn to values” in the sustainability literature. In this paper we explore the meaning and use of the term “sustainability-aligned values.” Following the 2022 IPBES Values Assessment we consider these as values that are crucial for shaping decisions that will help bring about sustainability. Our characterization of sustainably-aligned values assumes inherent pluralism because of diverse interpretations of sustainability and of pathways toward it. Nevertheless, a review of three bodies of literature suggests that there is considerable agreement about the kinds of values that align with sustainability. In particular, the nurturing of certain relational values is now widely seen as supportive of sustainability, including values regarding what matters in human interactions with nature (such as stewardship), and values regarding relationships between humans (such as collectivism). We proceed to pose critical questions about the proposition that certain values support sustainability. We ask whether this emerging body of thought is consistent with pluralist requirements to foster values diversity, whether an agenda to nurture values aligned with sustainability is actionable, and how mobilizing sustainability-aligned values entails addressing power imbalances.