Magnetoelectric composites have attracted extensive attentions due to the possibility of room temperature coupling effect between the ferroelectric and magnetic phases. We report the comparative study of structure, dielectric , ferroelectric, magnetic properties as well as coupling effect for (1- x )Mn 0.5 Zn 0.5 Fe 2 O 4 - x Ba 0.85 Sr 0.15 Ti 0.9 Hf 0.1 O 3 ((1- x )MZFO- x BSTHO) ( x = 0.2, 0.35, 0.5, 0.65, 0.8) composite ceramics prepared by combining coprecipitation process with sol-gel method. The X-ray diffraction result confirm bi-phase structure of the composites, without apparent chemical reaction generated between MZFO and BSTHO. The samples present relative density surface, the mean grain size is in the range of 1–2 μm, which increases slightly with the decrease of molar ratio . The dielectric constant and loss show non-monotonic variation with molar ratio. Temperature and frequency dependence of relaxation peaks are due to the relaxation polarization induced by interface, space charges and weakly bound ions. The peak of the dielectric constant disappears when x is larger than 0.5, while the loss peaks were still observed for all the samples. The remnant polarization increases with x decreasing while the leakage current decreases because the concentration of high-resistance BSTHO is increased. The sample with x = 0.20 shows the largest saturated magnetization of 54 emu/g while the maximal effective saturated magnetization for MZFO is larger than 80 emu/g, obtained at x = 0.65. The coupling coefficient decreases first and then increases, finally it decreases again with the increase of x . The maximal magnetoelectric coupling coefficient is 1420 μV/(cm.Oe), which is obtained for the sample at x = 0.65. The anomalous magnetic and coupling behaviors can be attributed to the strong interface interaction between MZFO and BSTHO.