Learning a skill has been demonstrated to relate to neural plasticity in both animal and human brains. Performing diabolo consists of different tricks and may cause brain structural changes associated with psychophysical functions. Therefore, the purpose of this study was to investigate gray matter (GM) and white matter (WM) changes associated with psychophysical functions induced by diabolo training in healthy subjects. Fourteen healthy right-handed male subjects were enrolled to receive the diabolo training. Whole brain T1-weighted images and diffusion tensor imaging (DTI) data were acquired from all subjects on a 3.0 T magnetic resonance scanner before and after the training. Voxel-based morphometry (VBM), surface-based morphometry (SBM), and voxel-wise DTI analysis were carried out to detect the GM volume, cortical thickness, and WM diffusion changes using T1-weighted image and DTI data, respectively. In addition, two-arm coordination and mirror-drawing tests were performed to evaluate their psychophysical functions before and after 2, 4, 6 and 8 weeks of training. Analysis of variance was performed to understand whether the psychophysical functions changed over time after the training. The results showed that the psychophysical functions were significantly changed over time during the training. The VBM and SBM analyses revealed that the GM volume and cortical thickness were significantly increased in the brain areas associated with visual, motor, sensory, and spatial cognition functions. The voxel-wise DTI analysis further demonstrated that the mean diffusivity was significantly reduced in the genu of corpus callosum. Moreover, significant correlations were revealed between the increase rate of GM volume and the improvement rate of psychophysical functions in the left angular gyrus. The results suggest that the diabolo training may induce increased GM volume associated with improved psychophysical function in the brain region involved in spatial cognition and attention. Therefore, we conclude that the diabolo training may improve psychophysical function which might be reflected by the increased GM volume in the angular gyrus.