In this chapter the reader is offered a critical introduction to the learning process in entrepreneurship and innovation development. It considers how learning enables the optimisation of the efforts of entrepreneurs and their search for innovative solutions to problems. This requires an understanding of the relationship between learning and entrepreneurship and how the different components of organisational, environmental and individual learning produce possibilities for entrepreneurial learning. The chapter engages the reader with novel approaches to entrepreneurial decision-making by individual entrepreneurs and organisations to develop competencies and capabilities for delivering innovative outcomes.