Polycrystalline Ba4Ni2−x Zn x Fe36O60 (0.0 ≤x ≤ 1.4) hexagonal ferrite samples have been prepared by conventional solid-state reaction method. Structural and magnetic properties of the prepared samples were then analyzed by the X-ray diffraction technique and with superconducting quantum interface device (SQUID) magnetometer, respectively. Variations of lattice parameters, density, and porosity with Zn content were measured. Magnetic properties such as complex permeability, relative quality factor, loss factor, and saturation magnetization have been investigated as a function of Zn content. The study revealed that Zn content has a significant effect on structural and magnetic properties of the Ba4Ni2Fe36 O 60 hexaferrites.