In this paper, Li0.43Zn0.27Ti0.13Fe2.17O4-xBaTiO3 composite materials (x = 0 wt%, 2 wt%, 4 wt%, 6 wt%, 8 wt%, 10 wt%) were prepared and the structure and properties were investigated. The result of X-ray diffraction (XRD) revealed that the composites contained two phase formations, with no other phases. Scanning electron microscopy (SEM) images showed that the size of grains decreased gradually with x increasing, and the densification was enhanced by adding BaTiO3 (BT) material. The magnetic permeability and dielectric permittivity of the samples were characterized. With increasing values of x, the real part of magnetic permeability μ decreased from 110 to 15 and the magnetic loss (tanδ μ ) remained at a low value. In addition, the real part of the dielectric permittivity increased first from 30 to 65 and then decreased after x = 6 wt%, and the dielectric loss (tanδ) reached the lowest value at x = 6 wt%. This material had a potential application in filter devices.