Synaesthesia is the involuntary physical experience of a crossmodal linkage such as when hearing a tone evokes the additional sensation of seeing a colour. We previously described a professional musician with absolute pitch perception who experiences both different tastes in response to hearing different tone intervals (e.g., major third and sweet) and the more common tone-colour synaesthesia in which each particular tone is linked to a specific colour (e.g., C and red). One of the current theories of synaesthesia proposes that local crossactivation or disinhibition of feedback occurs because of increased connectivity between relevant brain areas. Based on diffusion tensor and T1-weighted magnetic resonance imaging we performed fractional anisotropy (FA) analysis, probabilistic fibre tractography, and voxel-based morphometry in the synaesthete E.S. compared with 17 professional musicians and 20 normal control subjects using voxel-wise z-score transformations. We report increased FA and volumetric white (WM) and grey matter (GM) peculiarities in E.S.'s auditory and gustatory areas, hence explaining the interval-taste synaesthesia. Probabilistic fibre tractography revealed hyperconnectivity in bilateral perisylvian-insular regions in the synaesthete E.S. Differences in FA and volumetric WM and GM alterations in visual areas might represent the neuroarchitectural foundation of the tone-colour synaesthesia. Still unknown are the causes of the structural alterations, although an X-chromosomal linked dominant trait has been suggested. Whether hyperconnectivity occurs due to a failure in neural pruning or even synaptic sprouting remains to be shown. Our findings might have implications for the understanding of multimodal integration and may encourage similar research into dysfunctional perceptual phenomenon such as hallucinations in schizophrenics or in Charles Bonnet syndrome.