Post-mortem MRI provides the opportunity to acquire high-resolution datasets to investigate neuroanatomy, and validate the origins of image contrast through microscopy comparisons. We introduce the Digital Brain Bank (open.win.ox.ac.uk/DigitalBrainBank), an interactive data discovery and release platform providing open access to curated, multimodal post-mortem neuroimaging datasets. Datasets span three themes - Digital Neuroanatomist: data for neuroanatomical investigations; Digital Brain Zoo: data for comparative neuroanatomy; Digital Pathologist: data for neuropathology investigations. The first Digital Brain Bank release includes fourteen distinctive whole-brain diffusion MRI datasets for structural connectivity investigations, alongside microscopy and complementary MRI modalities. This includes one of the highest-resolution whole-brain human diffusion MRI datasets ever acquired, whole-brain diffusion MRI in seven non-human primate species, and one of the largest post-mortem whole-brain cohort imaging studies in neurodegeneration. Taken together, the Digital Brain Bank provides a cross-scale, cross-species investigation framework facilitating the incorporation of post-mortem data into neuroimaging studies.