The Tasmanian devil (Sarcophilus harrisii) is an endangered carnivorous marsupial confined to the island of Tasmania. Little is known about the structure and cellular organisation of the Tasmanian devil brain. We collected the brain of a 7-year-old Tasmanian devil that was euthanised for non-neurological reasons. The brain was hemi-dissected, and the right hemisphere was prepared for cryosectioning. It was serially sectioned and labelled with cresyl violet to create a coronal atlas. A challenge when studying the cellular architecture of marsupial tissue is a lack of antibodies to label different cell types. We therefore next assessed several commercially available antibodies to label cells of the neurovascular unit, a group of cells that together regulate cerebral blood flow (CBF). We successfully labelled astrocytes (GFAP), blood vessels (lectin), neurons (NeuN), pericytes (PDGFRβ) and microglia (lectin). Like all marsupials, we found that Tasmanian devil cerebral blood vessels display a unique paired structure, with pairs of arterioles and venules penetrating the brain and then branching in unison into a capillary network, before uniting at terminal capillary loop structures. Curiously, we observed PDGFRβ-positive cell soma within these capillary loops, which we hypothesise are pericytes, a contractile cell with roles in CBF regulation and blood-brain-barrier integrity. To the best of our knowledge this is the first description of this phenomenon. Collectively, our work enables a deeper understanding of Tasmanian devil brain cytoarchitecture which can be linked to behaviour, and we shed new light on the structure of marsupial capillary loop structures.