Highly crystalline and monodisperse cobalt ferrite nanocrystals were fabricated by the high-temperature aging of a metal-surfactant complex followed by mild oxidation. Particle sizes were varied from 4 to 9 nm by changing the experimental conditions. Transmission electron microscopic (TEM) images of the particles showed two-and three-dimensional assembly of the particles, demonstrating the uniformity of the nanocrystals. Electron diffraction, X-ray diffraction, and high-resolution transmission electron microscopic images of the nanocrystals confirmed the highly crystalline nature of the cobalt ferrite structure. The elemental analysis confirmed the stoichiometry of cobalt ferrite, despite some variations in the relative atomic composition of nanocrystals. The nanocrystals were found to have typical behaviors of magnetic nanocrystals and the narrow energy barrier distributions of magnetic anisotropy, implying that the nanocrystals obtained are very uniform.The development of uniform magnetic nanocrystals has been intensively pursued because of their applications in magnetic data storage, ferrofluids, medical imaging, drug targeting, and catalysis. 1,2 Recently, several metallic magnetic nanocrystals of uniform particle size have been fabricated. 3 Magnetic oxide nanocrystals having uniform particle size have been synthesized. 4,5 However, a very difficult size-selection process was required to obtain magnetic nanocrystals having uniform particle size distribution. Recently, we developed a new procedure for producing highly crystalline and monodisperse γ-Fe 2 O 3 nanocrystals without a size-selection process. 6 These iron oxide nanocrystals were synthesized from the controlled oxidation of uniform iron nanoparticles generated from the thermal decomposition of an iron-surfactant complex. We have extended the synthetic method to fabricate bimetallic oxide nanocrystals and report upon the synthesis of monodisperse and highly crystalline cobalt ferrite nanocrystals.In the synthetic procedure, uniform iron-cobalt alloy nanoparticles were first generated from the thermal decomposition of a metal-oleate complex and further oxidized to yield cobalt ferrite nanocrystals. The precursor, (η 5 -C 5 H 5 )CoFe 2 (CO) 9 , was prepared using the previously reported synthetic procedure. 7 A typical synthesis of cobalt ferrite nanocrystals with a particle diameter of 6 nm is as follows. A total of 0.2 g of (η 5 -C 5 H 5 )-CoFe 2 (CO) 9 (1.23 mmol; total metal atoms) was added to a mixture containing 5 mL of dioctyl ether and 1.04 g of oleic acid (3.69 mmol) at room temperature under an argon atmosphere. The mixture was heated to reflux (∼300°C) and kept at that temperature for 1 h. The color of the reaction mixture changed to clear blue at 230°C and to black at the reflux temperature. The blue color formed at 230°C seemed to be due to a metal oleate complex. The resulting black solution was cooled to room temperature, and 0.28 g of dehydrated (CH 3 ) 3 -NO (3.69 mmol) was added. The mixture was then heated to 130°C under an argon...