A burgeoning interest in the intersection of neuroscience and architecture promises to offer biologically inspired insights into the design of spaces. The goal of such interdisciplinary approaches to architecture is to motivate construction of environments that would contribute to peoples' flourishing in behavior, health, and well-being. We suggest that this nascent field of neuroarchitecture is at a pivotal point in which neuroscience and architecture are poised to extend to a neuroscience of architecture. In such a research program, architectural experiences themselves are the target of neuroscientific inquiry. Here, we draw lessons from recent developments in neuroaesthetics to suggest how neuroarchitecture might mature into an experimental science. We review the extant literature and offer an initial framework from which to contextualize such research. Finally, we outline theoretical and technical challenges that lie ahead.