A novel CNTs-based composite, LiZn ferrite (Li0.435Zn0.195Fe2.37 O4) coated CNTs core-shell nanostructure, was successfully prepared by a sol-gel method. The core-shell hetero-nanostructure have confirmed by TEM and XRD. The effect of surface oxidation treatment of MWNTs was investigated by FT-IR. The result showed that MWNTs functionalized with–COOH and –OH, etc. groups form an efficient matrix for the growth of LiZn ferrite crystals.