This article explores the potential of polycentric governance to strengthen civic virtue for collective action towards social-ecological sustainability, including by helping ‘re-enchant’ human relationships with the more-than-human world (Nature). Much of humanity remains alienated in some degree from Nature under the influence of a ‘disenchanted’ (anthropocentric) worldview rendering her of only instrumental value to us. The consequent loss of human affinity with Nature depleted the civic virtue required for this sustainability. The potential for polycentric governance to strengthen this virtue is explored by drawing from theories of collective action and self-determination, and from scholarship on biophilia, Indigenous knowledge, and non-human behaviour. This potential is affirmed in respect of community-based forms of this governance informed by the subsidiarity principle and Indigenous knowledge systems that Fikret Berkes identified as central to sacred ecology as a re-enchanted tradition of ecological science. The article concludes from an anthropocentric perspective that community-based, versus centralised, sustainability governance is likely to cultivate more civic virtue for sustaining Nature given its greater support for humans’ basic psychological needs. A sacred ecology perspective leads to the conclusion that such governance has potential to generate further such virtue by increasing our exposure to Nature and thereby strengthening fulfilment of these needs. The additional needs fulfilment arising from a re-enchanted worldview can thus lead us to care and act more for Nature – not only from enlightened recognition of the instrumental value of doing so but also from experiencing more of Nature as integral to our senses of self.