We evaluated the extent of laterality of the diffusion spectrum imaging (DSI) indices, and tested the association of their laterality to laterality of neurometabolite concentrations derived from whole-brain MR spectroscopic imaging (MRSI). Leftward asymmetry was observed mainly in the motor structures and rightward asymmetry in the structures associated with attention and emotion. A similar pattern of GFA, NQA and FA laterality in NAA/Cr and Cho/Cr and a reversed pattern in ADC were observed. The combination of DSI and MRSI can be helpful for a better understanding of ongoing neural processes. Hemispheric lateralization needs to be paid attention when interpreting pathologies.