The results of current investigation demonstrate that mechanochemical processing can be used to synthesize high purity Fe2B nanocrystals by selecting well-optimized milling conditions, reaction paths and proper starting materials. Microstructure, phase analyses, specific surface area, and magnetic properties of the synthesized nanocrystals were examined by using X-ray diffraction/spectroscopy, electron microscopy, nitrogen adsorption-desorption methods following Brunauer-Emmett-Teller equation and vibrating sample magnetometer techniques, respectively. Removal of MgO impurity phase by leaching the resulting powder in the acetic acid solution yielded single phase Fe2B nanocrystals with the crystallite size and specific surface area of 12.5 nm and 29 m(2)/g, respectively. Magnetization results clearly indicated the ferromagnetic behavior of Fe2B nanocrystals with saturation magnetization observed around 96.26 emu.g(-1). Electron microscope images revealed coaxial/spherical powder shape and morphology of the single-phase Fe2B nanocrystals. (C) 2017 The Society of Powder Technology Japan. Published by Elsevier B.V. and The Society of Powder Technology Japan. All rights reserved.