A series of Ni doped cobalt ferrite compounds with the formula Ni x Co 1−x Fe 2 O 4 where x=0, 0.2, 0.4, 0.6, 0.8, and 1.0 were prepared using a hydrothermal method and subsequently sintered/annealed at 600• C for 3 h. The influence of the Ni content on the lattice parameter, a, stretching vibration and the magnetization of specimens were subsequently studied. XRD and FTIR were used to investigate structure and composition variations. All samples were found to have a cubic spinel structure. SEM was used to study morphological variations. The results indicate that the average particle sizes are between 30-35 nm with a narrow size distribution along with nanocrystals forming of regular octahedrons. A decrease in the peak to peak line width and increase in resonance field with increasing Ni content were observed from ESR measurements. Based on ESR results, a core-shell type of formation was proposed where the core is made up of undoped CoFe 2 O 4 and the shell is Ni 2+ doped CoFe 2 O 4 .