A novel three-phase, double-percolating composite with a ferromagnetic phase (NiZn ferrite) and metallic inclusion (nickel) embedded in the polyvinylidene fluoride matrix is prepared by a simple hot-molding method. The large ferrite particles in the composite not only act as magnetic phase, endowing the composite with high initial permeability, but also present as a high-volume fraction discrete (nonpercolating) phase, confining polymer and metallic particles into a continuous double-percolating structure of low volume fractions. The increase in the content of the magnetic nickel particles compensates the decrease in the content of the NiZn ferrite, hence a stable initial permeability with an enhanced dielectric constant has been observed. The dielectric losses of the composites were reduced compared with the previous works.