We developed an approach to prepare the multilayered 3D composites where aligned multiwalled carbon nanotubes (MWCNTs) were grown on the surface of quartz fiber cloths (QFCs) by chemical vapor deposition method. The morphologies of the MWCNTs-QFCs preforms were analyzed by field emission scanning electron microscopy, transmission electron microscopy, and thermogravimetric analysis. The results showed that the growth of high yield and uniform alignment of MWCNTs on the surface of QFCs could be controlled by the process. The unique MWCNTs-QFCs preforms, when served as connecting bridges for structural epoxy composites, demonstrated a significant enhancement of the interlaminar shear strength and electrical conductivity along in-plane and out-of-plane directions when compared to QFCs/epoxy composites without MWCNTs, making the MWCNTs-QFCs reinforcements meaningful in structural composites.