A self-assembled Cu-Fe-Ni-Cr-Si immiscible composite with a bilayer structure was produced by laser induction hybrid cladding (LIHC) as a result of liquid phase separation (LPS). The microstructure exhibited by large amounts of ferromagnetic (FM) Fe3Si particles dispersed within the ε-Cu matrix in the upper layer, and many ε-Cu particles embedded within the FM Fe3Si matrix in the lower layer. The microhardness values of the Fe3Si matrix lower layer (758HV0.2) and ε-Cu matrix upper layer (248HV0.2) were ∼7.3 and ∼2.4 times higher than that of pure copper by LIHC, respectively, indicating that the immiscible composite exhibited strongly inhomogeneous characteristics consistent with a “bilayer structure”. Moreover, the immiscible composite showed a high saturation magnetization of 96.2 emu/g and a low coercivity of 7.24 Oe due to the formation of FM Fe3Si with micro- and nanoscaled structures. Display omitted •Composite consists of Cup embedded into Fe3Si matrix and Fep dispersed in ε-Cu matrix.•Immiscible composite exhibits a “bilayer microhardness”.•Immiscible composite has high saturation magnetization (96.2 emu/g).•Immiscible composite exhibits a low coercivity (7.24 Oe).