Magnetic nanoparticles of chromium substituted cobalt ferrite (CoFe2−xCrxO4) were prepared by the co-precipitation method for different concentrations (x=0.0, 0.1, 0.2 and 0.3) of chromium (Cr) and were annealed at 600°C for 3h. Formation of single phase cubic spinel structure was confirmed by X-ray diffraction analysis and the average crystallite size was in the range of 15–23nm. Studies on the energy dispersive spectroscopy confirm the presence of Cr in Cr substituted CoFe2O4 nanoparticles. Transmission electron microscopy observations revealed that CoFe2O4 and Cr substituted CoFe2O4 nanoparticles are uniformly distributed and not highly agglomerated. Dielectric properties such as dielectric constant (ε′) and dielectric loss (εʺ) of prepared nanoparticles were investigated as a function of frequency and temperature. The dielectric study reveals that dielectric constant and dielectric loss are higher for Cr substituted CoFe2O4 than the corresponding value of pure CoFe2O4 nanoparticles. Studies on magnetic properties revealed that the saturation magnetization of samples decreases with increasing Cr concentration and lies in the range of 69.67–42.71emu/g for the prepared samples. Strong red emission and weak blue and UV emissions are observed from the fluorescence spectral analysis of the prepared pure and Cr substituted CoFe2O4 nanoparticles.