We report on a novel ferroelectric/gyromagnetic ferrite layered composite thin film with two degrees of tuning freedoms. The structure was prepared by layered growth of Y3Fe5O12(YIG) ferrite, LaNiO3(LNO) electrode and (100) orientated Pb0.4Sr0.6TiO3 (PST) ferroelectric films on Si substrates by RF magnetron sputtering. LNO not only exists as an electrode, but also provides a buffer layer for the orientation growth of PST film. The PST/YIG composite thin films exhibited large magnetic tunability of μr (92.1%@600 Oe), low FMR linewidth (ΔH) of 160.7 Oe@9.1GHz and high electrical tunability (η) of 75%@360kV/cm, which shows potential applications in magnetically and electrically tuning devices.