The Ni1-xFexO (x = 0.00, 0.02, 0.04 and 0.06) nanoparticles are synthesized by chemical precipitation route using polyvinyl-pyrrolidone (PVP) and nitrate metal salts. The results of thermogravimetric analysis (TGA) of the synthesized dried hydroxide powders showed that thermal decomposition occurs up to 500 degrees C so as to form pure Ni1-xFexO. Therefore, all synthesized samples were calcined at 500 degrees C for 4 h and then used for further characterization. Energy dispersive X-ray spectroscopy (EDS) of all the samples showed the presence of Ni, O and Fe without any other impurities. From X-ray diffraction (XRD) and transmission electron microscopy (TEM) we could prove that the samples are polycrystalline in nature and are in single phase. The different vibrational modes in Ni1-xFexO (x = 0.00, 0.02, 0.04 and 0.06) nanoparticles were studied by Raman spectroscopy and Fourier transform infrared spectroscopy (FTIR). Further, we analyzed the optical response from ultraviolet visible spectra and Photoluminescence (PL) spectra.