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Two phase-based composites consisting of magnetic Mg0·6Cd0·4Co0·05Fe1·95O4ferrite and dielectric magnesium titanate (MgTi2O4) were synthesized through a solid-state route. The structural and high-frequency magneto-dielectric properties of a series of (Mg0·6Cd0·4Co0·05Fe1·95O4)1-x+(MgTi2O4)xwith xcontents of 0.00, 0.06, 0.12, and 0.18 were studied. The phase structure was examined via X-ray diffraction (XRD), the results indicated the occurrence of both spinel MgTi2O4and MgFe2O4phases in various composites. Meanwhile, grain size and bulk density were lowered with the introduction of MgTi2O4, which also significantly weakened magnetic properties with decreased saturation magnetization (Ms) from 43.05 emu/g to 20 emu/g and coercivity (Hc) from 67.02 Oe to 3.35 Oe. In addition, the real permeability (μʹ) decreased and permittivity (ε′) increased with increasing MgTi2O4content over the wide frequency range of 0.5–5 GHz. Finally, a low order of magnitude (tan δμ ≈ 10−1to 10−2and tan δε ≈ 10−2to 10−3) was obtained for all composites. These results demonstrated that the synthesized composites were expected to be an ideal candidate for high-frequency antenna loading materials.