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There are approximately 85,000 people in prisons in England and Wales, presenting with a high prevalence of complex health needs. Although the primary aim of incarceration is not health improvement, prisons provide an opportunity for health services to access a hard-to-reach and underserved population. Health Literacy has gained increasing prominence as a field of study and has been identified as a key determinant of health. At its core, it describes the process by which individuals are actively involved in and in control of their own health. The links between poor health literacy and substantial health consequences is well established, however, the relevance to prison settings and prison populations is less clear. This study therefore aimed to examine Health Literacy in a prison setting. Health Literacy and other health outcome measures were administered to 104 prisoners in a single prison setting. The study demonstrated that 75% held limited Health Literacy compared with 15% in a comparable community population sample. Limited health literacy was related to increased anxiety and depression scores and negative affect and intentions to quit smoking. This research highlights the particular challenges faced by prisons in promoting Health Literacy and makes recommendations for developing a health literate prisons concept.