Multiferroic BiFeO3 (BFO) thin films exhibit both ferroelectric and ferromagnetic properties at room temperature, and have broad potential applications in the field of multifunctional electronic devices. Here, 2-2 type Bi0.89Tb0.11Fe0.96Mn0.02Co0.02O3/Zn1-xCuxFe2O4 (BTFMCO/ZCxFO, x = 0, 0.5) thin films were successfully prepared on FTO substrates by the sol-gel method, and the effects of the ZCxFO magnetic layer on the structural, surface morphological, dielectric, ferroelectric and ferromagnetic properties of the thin films were investigated. The results show that the saturation polarization intensities of the BTFMCO/ZFO thin film and the BTFMCO/ ZC0.5FO thin film are 60 mu C/cm2 and 82 mu C/cm2, respectively, and the saturation magnetization intensities are 36.5 emu/cm3 and 66.1 emu/cm3, respectively. After doping the magnetic layer, both the ferroelectricity and ferromagnetism are significantly enhanced simultaneously. These superior multiferroic properties provide new opportunities for the development of innovative multifunctional electronic components.