Thermodynamic modeling of the Ni 0.5 Zn 0.4 Cu 0.1 Fe 2 O 4 complex ferrite system has been adopted as a rational approach to establish routes to better synthesis conditions for pure phase Ni 0.5 Zn 0.4 Cu 0.1 Fe 2 O 4 complex ferrite. Quantitative analysis of the different reaction equilibria involved in the precipitation of Ni 0.5 Zn 0.4 Cu 0.1 Fe 2 O 4 from aqueous solutions has been used to determine the optimum synthesis conditions. The spinel ferrites, such as magnetite and substitutes for magnetite, with the general formula MFe 2 O 4 , where M= Fe 2+ , Co 2+ , and Ni 2+ are prepared by coprecipitation of Fe 3+ and M 2+ ions with a stoichiometry of M 2+ /Fe 3+ = 0.5. The average particle size of the as synthesized Ni 0.5 Zn 0.4 Cu 0.1 Fe 2 O 4 , measured by transmission electron microscopy (TEM), is 14.2 nm, with a standard deviation of 3.5 nm the size when calculated using X-ray diffraction (XRD) is 16 nm. When Ni 0.5 Zn 0.4 Cu 0.1 Fe 2 O 4 ferrite is annealed at elevated temperature, larger grains are formed by the necking and mass transport between the Ni 0.5 Zn 0.4 Cu 0.1 Fe 2 O 4 ferrite nanoparticles. Thus, the grain sizes of the Ni 0.5 Zn 0.4 Cu 0.1 Fe 2 O 4 gradually increase as heat treatment temperature increases. Based on the results of Thermogravimetric Analysis (TGA) and Differential Scanning Calorimeter (DSC) analysis, it is found that the hydroxyl groups on the surface of the as synthesized ferrite nanoparticles finally decompose to Ni 0.5 Zn 0.4 Cu 0.1 Fe 2 O 4 crystal with heat treatment. The results of XRD and TEM confirmed the nanoscale dimensions and spinel structure of the samples.