The effect of Sr2+ ions on the microstructure and high frequency properties of 2.5 wt% Bi2O3 added to Co(2)Z hexaferrites (3Ba(1-x)SrxO•2CoO•12Fe2O3, x = 0.0, 0.2, 0.4 and 0.6) synthesised using the solid-state reaction method was investigated. Experimental results indicate that the dielectric properties were markedly enhanced with the increase in the content of Sr2+ ions, thereby increasing the miniaturisation factor, which enables a size reduction in a long frequency range. Slight changes to saturation magnetisation (Ms) and coercivity (Hc) were observed, i.e., the saturation magnetisation (Ms) decreased from 39.99 to 38.11 emu/g, and coercivity (Hc) increased from 59.05 to 65.21 Oe when x increased from 0.0 to 0.6. Meanwhile, ε′ increased from approximately 8 to 12, indicating the invariability in μ′. In addition, the processed materials exhibit relatively low magnetic loss and dielectric loss (magnetic loss tanδμ ≈ 0.08 and dielectric loss (tanδε ≈ 0.007)). These results indicate that the substituted CO(2)Z ferrites have excellent potential in high-frequency antenna applications.