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The amorphous of Permalloy on the copper subtract was studied using composite electroplating method. A portion of hydrogen brings the counteraction on the surface of cathode leading nickel-iron alloys to be anomalous in the process of co-depositing. The results of X-ray diffraction (XRD) show that the Ni-Fe alloys layer is amorphous. The Giant Magneto -Impedance (GMI) effect of Ni-Fe alloys was obtained under the optimal conditions, dependence on the soft magnetic property of Ni-Fe amorphous thin film. As a result, the ratios△ Z/Z of NiFe/Cu/NiFe amorphous thin film are 30% at 40 kHz which is in low frequency. Furthermore, the GMI value of NiFe/Cu/NiFe amorphous thin film with a sandwich structure is higher than that of single-layer ferromagnetic films of the same thickness.