In this study, amorphous FeB alloy modified magnetitenanocomposites (Fe 3 O 4-FeB) were facilely synthesized by interfacialreduction of commercialFe 3 O 4 nanoparticles with NaBH 4. TEM, CS-STEM integrated with EDS, Mössbauer spectroscopyanalysis confirmed the formation of Fe 3 O 4-FeB, where a shell of amorphous FeB nanoparticles with 2-4 nm in size was surrounded on the inner magnetite Fe 3 O 4 part.Fe 3 O 4-FeB displayed a promotedCr(VI)removal efficiency compared withthe bare Fe 3 O 4 counterpart, the interfacial reduced Fe 3 O 4 nanoparticles with hydrogen and/or with hydrazine hydride. XPS analysis evidenced that reduction of Cr(VI) on surface of the Fe 3 O 4-FeB was the major contribution to the Cr(VI) removal. Tafel polarization analysis of the Fe 3 O 4-FeB and aqueous boron speciesmeasurement indicated thathigh Cr(VI) removal efficiencywith Fe 3 O 4-FeB was highly depended on amorphous FeB alloy shell, in which boron element containing free electrons could accelerate the electron transfer from Fe to the adsorbed Cr(VI), as well reduce Fe(III) to Fe(II) and thus promote the Fe(III)/Fe(II) cycles.The efficient Cr(VI) removal under a wide range of pH values and its easy magnetic separationmake the Fe 3 O 4-FeB be a potential for Cr(VI) contaminated water