Graphene (Gr), a well-known 2D material, has been under intensive investigation in the last decade due to its high potential applications in industry and advanced technological elements. The Gr, while composed with magnetic materials, has opened new opportunities for further developments of magnetic based devices.Here, we report a mass production of Gr/Ni composite powders using electrochemical exfoliation/deposition method with different magnetic strengths of the final composite material. We applied the magnetic composite materials in a magnetoimpedance (MI) based sensor and observed significant enhancement in the MI effect and its field sensitivity. Such magnetic composites with controlled magnetization strengths are coated on the MI-ribbon sensor surface and different MI responses are observed. The MI response of a ribbon coated with a Gr/Ni layer is theoretically determined based on an electrodynamic model with a qualitative consistency between the experimental results and the theoretical model. Our comprehensive study can be applied in high performance functionalized MI based magnetic sensors and devices.