Magnetoelectric composites have attracted widespread attention during the past few decades due to their strong magnetoelectric coupling effect and potential applications above room temperature. Ni 0.5 Zn 0.5 Fe 2 O 4 /Ba 0.8 Sr 0.2-TiO 3 composites have been prepared by the conventional high-temperature solid-state method and the effects of Al 2 O 3 addition on their microstructure, dielectric, ferroelectric, and magnetic properties studied. x-Ray diffraction (XRD) analysis confirmed the biphase structure of the composites. scanning electron microscopy (SEM) showed that addition of a certain amount of Al 2 O 3 can enhance the density and promote uniform growth of particle size. The sample with 1 wt.% Al 2 O 3 addition exhibited the largest dielectric constant and lowest dielectric loss (< 0.05 at 1 kHz) at high temperature (> 354°C). The sample with 3 wt.% Al 2 O 3 addition presented the best ferroelectric properties, with the highest values of residual polarization (P r = 2.2150 lC/ cm 2 ) and coercive field (E c = 30.6527 kV/cm) among the specimens. The remanent magnetization (M r ) and saturated magnetization (M s ) decreased with increasing Al 2 O 3 content. In short, addition of Al 2 O 3 caused changes in the grain size, density, and defects, and addition of a certain amount of Al 2 O 3 can improve the magnetoelectric properties.