This article provides a new consideration of how Thomas Willis (1621–75) came to write the first works of ‘neurology’, which was in its time a novel use of cerebral and neural anatomy to defend philosophical claims about the mind. Willis’s neurology was shaped by the immediate political and religious contexts of the English Civil War and Restoration. Accordingly, the majority of this paper is devoted to uncovering the political necessities Willis faced during the Restoration of the English monarchy in 1660, with particular focus on the significance of Willis’s dedication of his neurology and natural philosophy to the Archbishop of Canterbury, Gilbert Sheldon. Because the Restoration of Charles II brought only a semblance of order and peace, Willis and his allies understood the need for a coherent defense of the authority of the English church and its liturgy. Of particular importance to Sheldon and Willis (and to others in Sheldon’s circle) were the specific ceremonies described in the Book of Common Prayer, a manual that directed the congregation to assume various postures during public worship. This article demonstrates that Willis’s neurology should be read as an intervention in these debates, that his neurology would have been read at the time as an attempt to ground orthodox worship in the structure of the brain and nerves. The political necessities that helped to shape Willis’s project also help us to better understand Willis’s innovative insistence that philosophical statements about the mind should be formulated only after a comprehensive anatomical investigation of the brain and nerves.