Composite structure materials were potential sensing elements for magnetic sensors due to Giant magnetoimpedance (GMI) effect. Two kinds of composite wires with different magnetic/non-magnetic structures were fabricated by using electroless deposition methods and the magnetoimpedance properties were investigated. The maximum GMI ratio of 114% was acquired at 60 MHz in the composite wires with a ferromagnetic core, whereas, 116% of maximum GMI ratio was found in the composite wires with a conductive core at low frequency of 600 kHz. These results exhibit that the GMI ratio reaches the maximum when magnetoresistance ratio ∆R/R and magnetoinductance ratio ∆X/X make the comparative contributions to the total magnetoimpedance (MI). The obvious GMI effect obtained in the composite wires with conductive core frequency may provide a candidate for applications in magnetic sensors, especially at low frequencies.