Gadolinium-substituted cobalt manganese ferrite nanoparticles with the composition Co0.6Mn0.4GdxFe2-xO4 (where x ranges from 0.0 to 0.08, with x = 0.02) were prepared through the sonochemical method. X-ray diffraction reveals that grown samples are single-phase cubic spinel belonging to space group Fd3m, where the crystallite sizes decrease with increasing Gd3+ content. At high doping ratios (x > 0.06), there was a slight increase in crystallite size compared to that of pure Co-Mn ferrite (x = 0), while the lattice parameter (a) decreased in the low doping range of Gd (x < 0.06), resulting in a reduction in crystallite size. Bertaut’s method confirms that 80% of the tetrahedral (A) sites were occupied by Mn ions, while the remaining sites were occupied by other cations in the octahedral (B) positions. Gd3+ ions were found exclusively in the octahedral-B sites. Co2+ ions were expected to occupy the octahedral-B site, which was confirmed in this study for the x = 0.0 and 0.02 samples. Field emission scanning electron microscopy shows the samples are agglomerated and have dense structures. Fourier transform infrared and Raman spectra validated the presence of spinel ferrite modes. Dielectric investigations indicate that as the Gd3+ content exceeds x = 0.0, the dielectric constant and dielectric loss decrease at lower frequencies. The observed dielectric behavior exhibited typical dispersion patterns attributed to Maxwell-Wagner polarization. Furthermore, changes in dielectric properties were observed as the Gd3+ content in Co0.6Mn0.4GdxFe2-xO4 nanoparticles increased, which can be attributed to the presence of oxygen vacancies and variations in the distribution of Fe3+ ions at both A and B-sites.