Addressing the biodiversity crisis requires renewed collaborative approaches. Large carnivores are ambassador species, and as such they can aid the protection of a wide range of species, including evolutionarily distinct and threatened ones, while being popular for conservation marketing. However, conflicts between carnivores and people present a considerable challenge to biodiversity conservation. Our cross disciplinary essay brings together original research to discuss key issues in the conservation of large carnivores as keystone species for biodiversity rich, healthy ecosystems. Our findings suggest the need to promote coexistence through challenging ‘wilderness’ myths; to consider coexistence/conflict as a continuum; to include varied interest groups in decision making; to address fear through positive mediated experiences, and to explore further partnerships with zoos. As wide-reaching institutions visited by over 700 million people/year worldwide, zoos combine knowledge, emotion and social context creating ideal conditions for the development of care towards nature, pro-environmental behaviors and long-term connections between visitors and carnivores. Based on current research, we provide evidence that large carnivores and zoos are both powerful catalysts for public engagement with biodiversity conservation, recognizing barriers and suggesting future ways to collaborate to address biodiversity loss.