Despite an underlying assumption that, at least on some level, our environments influence what we do, a review of the literature on formal education reveals that empirical research on relations between the physical environment and learning is surprisingly sparse. Conducted as ethnography, this study examines learning activity in an open, flexible and digitally connected learning environment. It draws on 549 hours of observation over a nine-month period in a refurbished space designed to accommodate 181 year five and six students and their team of seven teachers, using one-to-one mobile computing. Observation was informed by sociomaterial theories of learning, theories of material ecology from anthropology and archaeology, and the framework for Activity Centred Analysis and Design (ACAD) from the learning sciences. Through theoretical reflection, I consider how the qualities of materials participate in teaching and learning practice, and how we might account for their participation in learning activity. The theoretical exposition, housed in Part 1, traverses three scale levels: the qualities and properties of materials, the relational dependences between things and humans, and the notion of emergent, systemic wholeness. Part 1 concludes with the identification of a number of repeating patterns of structure and activity that give rise to wholeness, which are presented in the form of a partial pattern language. All of this draws on ten rich descriptions of learning activity, presented in Part 2. Throughout, I argue that there is an urgent need for a non-deterministic theory of materials in educational research, and that this type of detailed observational work can play a vital role in understanding how vibrant and participatory learning environments function and evolve. As such, this thesis makes both theoretical and practical contributions that have implications for teachers and educational leaders who wish to engage in shaping convivial places for learning