This chapter begins with the assertion that an Arts-led literacy curriculum is imperative if today’s students are to leave school with a sense of their own identity and a place within their social world, along with the creative and flexible literacy skills needed for life in the twenty-first century. Embedding the Arts in formal literacy learning contexts enables educators to enhance students’ imaginative capacities. This is central to student learning because, as Wordsworth (in Egan 1992: 25) proclaimed, imagination is ‘reason in her most exalted mood’. Kieran Egan’s Imaginative Research in Education (IERG) website reminds us that imagination is ‘the ability to think of the possible, not just the actual, it is the source of invention, novelty and flexibility in human thinking …it greatly enhances rational thought’. Initially this chapter provides a definition of how the term ‘the Arts’ should be understood for this discussion. A brief justification for the role of the Arts in imaginative learning follows, specifically in relation to the literacy curriculum and drawing on a range of relevant research and literature. Finally, two recent exemplars of Arts-led literacy programmes with primary students demonstrate the power of such curriculum experiences.