Saturation magnetization, magneto-crystalline anisotropy field and dielectric properties are closely related to microwave devices applied at different frequencies. For regulating the magnetic and dielectric properties of W-type barium ferrites, single-phase BaMe
2Fe16O27 (Me = Fe, Mn, Zn, Ni, Co) with different Me ions were synthesized by the high-temperature solid-state method. The saturation magnetization (M
s) range from 47.77 emu/g to 95.34 emu/g and the magnetic anisotropy field (H
a) range from 10700.60 Oe to 13739.57 Oe, depending on the type of cation substitution in the hexagonal lattice. The dielectric permittivity and dielectric loss decrease with increasing frequency of the AC electric field in the low-frequency region, while they almost remain constant in the high-frequency region. The characteristics of easy regulation and preparation make it a potential candidate for use in microwave device applications.