Nanocrystalline nickel-zinc substituted chromium ferrites having the chemical formula Ni_0.6Zn_0.4Cr_xFe_2-xO_4, i.e., NZCrF (where x= 0.0, 0.2, 0.4, 0.6, 0.8 and 1.0 wt.%) have been synthesized by flash auto combustion method. Consequently, preparation and characterization of Ni_0.6 Zn_0.4Cr_0.6 Fe_1.4O_­4 doped Polyvinyl alcohol (PVA)/Rhodamine dye nanocomposites using solvent casting technique have been reported. The X-ray diffraction (XRD) and Fourier-transform infrared spectroscopy (FTIR) studies confirm polymer nanocomposites' formation through the interaction between the nanoparticles and the polymer. Transmission electron microscope (TEM) and scanning electron microscope (SEM) images have investigated surface morphology and particle orientation. The average grain size is estimated to be approximately 51 nm. Images taken with TEM reveal that the composite Ni_0.6Zn_0.4Cr_xFe_2-xO_­4/PVA morphology is highly agglomerated, suggesting magnetic nanoparticles are encased in the PVA polymer chains. This may be due to the interaction between the ferrite's oxygen atoms and the PVA's polymer chains. The saturation magnetization (M_s), remnant magnetization (M_r), and coercivity (H_c) measured by VSM have been studied. The modification of PVA/Rhodamine dye nanocomposites with Ni_0.6Zn_0.4Cr_0.6Fe_1.4O₄ reveals their potential for usage in luminescence applications due to an improvement in the composites' optical characteristics.