Multiferroic ceramics with extraordinary susceptibilities coexisting are vitally important for the multi-functionality and integration of electronic devices. However, multiferroic composites, as the most potential candidates, will introduce inevitable interface deficiencies and thus dielectric loss from dissimilar phases. In this study, single-phased ferrite ceramics with considerable magnetic and dielectric performances appearing simultaneously were fabricated by doping target ions in higher valence than that of Fe3+, such as Ti4+, Nb5+ and Zr4+, into BaFe12O19. In terms of charge balance, Fe3+/Fe2+ pair dipoles are produced through the substitution of Fe3+ by high-valenced ions. The electron hopping between Fe3+ and Fe2+ ions results in colossal permittivity. Whilst the single-phased ceramics doped by target ions exhibit low dielectric loss naturally due to the diminishment of interfacial polarization and still maintain typical magnetic properties. This study provides a convenient method to attain practicable materials with both outstanding magnetic and dielectric properties, which may be of interest to integration and multi-functionality of electronic devices.