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Polycrystalline Ni–Zn–Cr ferrite nanoparticles with composition Ni0.5Zn0.5CrxFe2-xO4 (for x in the range of 0.00–0.25 insteps of 0.05) were prepared through the nitrate-citrate gel autocombustion method. The as-obtained powders were ground and annealed at 1000°C for 4 h and characterized for spinel phase using X-ray diffraction, transmission electron microscopy (TEM) and scanning electron microscopy (SEM). X-ray diffraction revealed the existence of single phase spinel while the TEM micrographs showed the presence of nearly spherical particles with soft agglomeration. Pelleted and toroidal samples of the same ferrite compound were sintered at 1000°C for 4 h. The dielectric constant and the dielectric loss tangent decreased with frequency in the range of 1 kHz–13 MHz while the initial permeability remained almost constant at lower measuring frequencies and thereafter increased with frequency for all samples. The observed variations have been discussed in the light of existing understanding.