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The vast majority of high-mobility organic semiconductors appear to be crystalline or at least semicrystalline, and grain boundaries between crystalline domains drastically affect charge transport in devices. Despite the acknowledged importance of domain structure and grain boundaries, until recently few experimental studies have been employed to examine their nature. On page 909 of this issue, Christopher McNeill reviews the last five years of progress with the range of diverse experimental approaches that have been used to image domain orientation and molecular order in organic semiconductor films, including optical, soft X-ray, electron and scanning-probe microscopies. These approaches are beginning to provide detailed information about the nature of sub-micron domain structure, and facilitating direct correlation with charge-transport physics.