Polypyrrole (PPY)/SrFe12O19 Composites with tunable electrical and magnetic properties were synthesized by in situ polymerization of pyrrole in the presence of SrFe12O19 particles. The structure of PPY/SrFe12O19 composites was characterized by means of Fourier transform infrared spectroscopy and X-ray diffraction. Transmission electron microscope and scanning electron microscope images illustrated that the spherical composites consisted of SrFe12O19 hexagonal plates sheathed by PPY. In the electromagnetic measurments, it was found that the ac conductivity of SrFe12O19 particles increased while the saturation magnetization, remanent magnetization, and coercivity decreased after PPY coating; moreover, the desired electrical and magnetic properties of PPY/SrFe12O19 composites can be modulated simply by controlling the contents of SrFe12O19 particles. A possible mechanism was also proposed to interpret the formation of the PPY/SrFe12O19 composites.