During the 1920s and 1930s, the British surgeon Geoffrey Keynes (1887–1982) treated breast cancer with radium instead of the hegemonic radical mastectomy, while vehemently attacking the “radicalists” for mutilating women. Keynes was also a leading bibliographer of literary figures from Sir Thomas Browne to William Blake through Jane Austen. This article argues that these endeavors did not inhabit separate worlds, but rather his bibliographic methods of collecting and sorting were deeply interwoven with his therapeutic practices and medical ways of knowing. The article also examines the profound influence his engagement with the works of William Blake had on his battle against the reigning medical orthodoxy and on the humanity of his relationship with his patients. It concludes that Keynes’ story sheds light on a now distant medico-cultural world where literary studies, often centered on book collecting and critique, were not only highly valued, but were influential in guiding the vision and behavior of a number of physicians.