© 2021 Elsevier Ltd and Techna Group S.r.l.This paper delineates a single-step production method of nanostructured diiron boride (Fe2B) and its structural, magnetic and magnetothermal properties. Structurally Fe2B resembles the tetragonal copper aluminide, CuAl2. The samples of nanostructured Fe2B were synthesized by milling Fe and B powders without any pre-treatment. Single phase Fe2B nanoparticles were successfully produced with the crystallite sizes of 68 and 46 nm after milling the powders for 10 h and 20 h, respectively. The saturation magnetization of the samples was found to decrease with increased milling time indicating that the surface spin disorder plays a crucial role in the magnetic properties. The highest saturation magnetization (Ms) of 141 emu/g with low coercivity (Hc) of 48 Oe was obtained for the 10 h milled sample of Fe2B, whereas the 20 h milled sample exhibited Ms and Hc as 129 emu/g and 149 Oe. This paper also presents a detailed information on the total and atom projected densities of state functions as well as the magnetic moment contribution of the individual atoms of Fe and B in Fe2B explaining the strong room temperature ferromagnetic properties contributed by the large number of unpaired 3 d electrons in Fe. The magnetothermal properties of the as-made Fe2B nanocrystals of high magnetic moment were investigated by measuring the rise in temperature as a function of time in the presence of AC magnetic fields. The magnetic Fe2B nanocrystals show significant thermal response with the high specific absorption rate of 172 W/g, demonstrating the advantages of using Fe2B nanocrystals for the application in magnetic fluid therapy for hyperthermia.