Hybridization of nanostructures opens new avenues for the synthesis of nano-architectures with multi-function and novel physicochemical properties. In this paper, we developed nanosphere template assisted physical vapor deposition to fabricate ordered multi-layered nanostructures utilizing Ag/dielectrics/CoFeB/dielectrics/Ag nanostructural arrays as examples. The structure dependent properties such as magnetic and optical properties are characterized. These nanostructures have distinct magnetic anisotropy being easier to saturate along the direction in the plane of the film. The adding of Ag makes the saturation magnetization (Ms) of nanostructure films decrease, and the coercive force (Hc) of various structural films increase. The correlation of the magneto-optical Kerr effect and the structure of the hybrid nanostructures are also investigated. It is found that Kerr effects can be greatly increased by addition of the nanostructural Ag layer and the dielectric layer.