The (Na0.5Bi0.5)0.98Ce0.02(Ti0.99Fe0.01)O3–BiFe0.95Mn0.05O3 (NBTCeFe–BFOMn) solid-solution thin film was fabricated on LaNiO3/Si substrate by metal organic decomposition. The leakage current density of NBTCeFe–BFOMn film at 400 kV/cm was reduced by approximately two orders of magnitude by reducing the density of oxygen vacancies and forming the defect complexes, compared with Na0.5Bi0.5TiO3 film. Much enhanced ferroelectric and magnetic properties were achieved in NBTCeFe–BFOMn film with a remanent polarization of 32.6 μC/cm2 and a saturated magnetization of 6.2 emu/cm3. The dielectric constant–voltage curve coincides well with the polarization–electric field loop.