In the present study, a facile one-pot synthetic route, utilizing a strong polar organic solvent, N-methyl 2-pyrrolidone (NMP), is demonstrated to obtain highly monodispersed ferrite nanocrystals. The equimolar mixture of oleic acid, C(17)H(33)COOH (R-COOH), and oleylamine, C(18)H(35)NH(2) (R'-NH(2)), was used to coat the magnetic nanocrystals. Structural and magnetic properties of the ferrite nanocrystals were studied by a multitechnique approach including X-ray diffraction (XRD), high resolution transmission electron microscopy (HRTEM), Fourier transform infrared (FTIR) spectroscopy, thermogravimetric analysis (TGA), X-ray photoelectron spectroscopy (XPS), vibrating sample magnetometry (VSM), and Mossbauer spectroscopy. FTIR spectral analysis indicates oleyiamine helps in deprotonation of oleic acid, resulting in the formation of an acid base complex, R-COO:NH(3)(+)-R', which acts as binary capping agent. Structural and coordination differences of iron were studied by XPS and Mossbauer spectral analysis. XPS analysis was carried out to examine the oxidation state of iron ions in iron oxide nanocrystals. The presence of a magnetically dead layer (similar to 0.38 and similar to 0.67 nm) and a nonmagnetic organic coating (similar to 2.3 and similar to 1.7 nm) may substantially reduce the saturation magnetization values for CoFe(2)O(4) and Fe(3)O(4) nanocrystals, respectively. The energy barrier distribution function of magnetic anisotropy was derived from the temperature dependent decay of magnetization. A very narrow energy barrier distribution elucidates that the ferrite nanocrystals obtained in this study are highly monodispersed.