The human brain relies upon the dynamic formation and dissolution of functional networks to support ongoing cognition. The goal of this study is to establish a relationship between functional and structural networks. Using ultra-high field MRI, structural network defined by grey matter myelination is measured via quantitative Magnetization Transfer. Magnetoencephalography (MEG) was used to elucidate functional networks representing the major electrophysiological pathways of communication in the brain. Our study sheds new light on the way in which cortical microstructure supports functional networks.