In this paper, we perform an integration between the tape casting and magnetron sputtering techniques to produce hybrid materials. To this end, trilayered nanostructures of NiFe/Cr/NiFe based on $$\hbox{Al}_{2}\hbox{O}_{3}$$ Al2O3 flexible sheet are produced by magnetron sputtering deposition. From the well-known dependence of the magnetic properties of NiFe alloy as a function of the thicknesses, here we study samples where the NiFe thicknesses are varied from 105.0 nm up to 142.5 nm, while the Cr layers varied from 15.0 nm up to 90.0 nm. From the structural characterization, a polycrystalline behavior for the $$\hbox{Al}_{2}\hbox{O}_{3}$$ Al2O3 grains dispersed in an amorphous matrix and a (111) orientation for the NiFe layers are observed. The magnetic characterization reveals the mirroring of the studied trilayered nanostructures concerning the traditional studies for the same thicknesses grown onto rigid (glass) substrate. These results bring these hybrid nanostructures as an attractive candidate for a flexible non-magnetostrictive material to use in smart and nano-functionalized ceramic materials.