The study of magnetic nanostructures is interesting because of its applications. Some of them are the development of magnetic refrigerators, ferrofluids, drug delivery systems, fabrication of devices with giant magnetoresistance effects, and high-frequency transformers. The physical and chemical properties of metal changes due to silica coating. The interaction potential can be manipulated using surface coatings and also the particle shape can be controlled. Nanoparticles with a proper surface coating are of interest for several other applications in optoelectronic devices and in the biomedical field. Thus, developing a new synthetic route for these particles and investigating the stability of magnetic materials are of great importance. Silica coating improves the chemical stability and electrical resistivity of the material. In this study, Ni3Fe (core) nanoparticles were prepared and the silica shell for this core was synthesized. The as-prepared X-ray diffraction (XRD) patterns and 300∘C annealed sample of Ni3Fe/SiO2 shows a characteristic hump in the low angle range confirming the presence of amorphous cristobalite phase of SiO2. The size of the Ni3Fe cluster in the Ni3Fe/SiO2 composite was estimated to be 8[Formula: see text]nm and 9[Formula: see text]nm, respectively, for the as-prepared and annealed samples. Vibrating sample magnetometer (VSM) measurements show the Ni3Fe to silica ratio to be 59:41. A small decrease in the coercivity value, is probably due to morphological changes associated with the coating. Scanning electron microscope (SEM) studies of the as-prepared and annealed Ni3Fe/SiO2 powder particles are of flowerlike morphology and in agglomeration. The impedance spectra were found at room temperature for the as-prepared samples.