Recent Catholic social thought features a consistent concern with the environment and humankind’s place in it. The natural world is a source of value and values. Pope Francis’s Laudato Si′ marks both continuity with extant Catholic Social Thought on the environment, and an advance growing out of it. The continuity is remarkable in Pope Francis’s recurrent critique of aspirations to technological mastery. The advance lies in a profound ethics of attunement that challenges not just present, weak environmental regulations, but also the dominant political and economic orders that enframe nature as little more than a pool of resources for human use and enjoyment. This essay explores the continuity between Laudato Si′ and Pope Benedict’s perspectives on environmental topics, explaining how Pope Francis’s Laudato Si′ has now complemented extant Catholic critique of value-free mastery with a profound account of attunement—that is, the fit between human nature and the natural world we are part of.