In this work, we adopted two sputtering modes to prepare the NiFe/Cu composite wires: (i) the intermittent deposition mode; and (ii) the continuous deposition mode. SEM images confirmed that the intermittent deposition mode leads to interface creation among deposited layers. XRD results showed that the intermittently deposited sample has a better crystallite and a grain growth. GMI effect has been used as a tool to analyze the magnetic properties of the samples. The results showed that the sputtered magnetic layers exhibit good soft magnetic properties, and the composite wires showed large GMI effect. The MI profile for the intermittently deposited composite wire shows two peaks, which can be a result of the different magnetic properties of the inner and the outer magnetic layers. The inherent stresses are partially relaxed through heat treatment. The GMI effect of the composite wire is enhanced, and the magnetic properties of the two magnetic layers become similar.