Polycrystalline gadolinium (Gd) substituted cobalt ferrites (CoFe 2-x Gd x O 4 ; x=0-0.3, referred to CFGO) ceramics have been synthesized by solid state reaction method. Chemical bonding, crystal structure and magnetic properties of CFGO compounds have been evaluated as a function of Gd-content. X-ray diffraction and Raman spectroscopic analyses confirmed the formation of inverse spinel structure. However, a secondary ortho-ferrite phase (GdFeO 3 ) nucleates for higher values of Gd-content. A considerable increase in the saturation magnetization has been observed upon the initial substitution of Gd (x=0.1). The saturation magnetization drastically decreases at higher Gd content (x≥0.3). No contribution from ortho-ferrite GdFeO 3 phase is noted to the magnetic properties. The increase in the magnetic saturation magnetization is attributed to the higher magnetic moment of Gd 3+ (4f 7 ) residing in octahedral sites is higher when compared to that of Fe 3+ (3d 5 ) and as well due to the migration of Co 2+ (3d 7 ) ions from the octahedral to the tetrahedral sites with a magnetic moment aligned anti-parallel to those of rare earth (RE 3+ ) ions in the spinel lattice. Increase in coercivity with increase in Gd 3+ is content is attributed to magnetic anisotropy in the ceramics.