We present an efficient approach for chemoselective synthesis of various functionalized arylamines from nitroarenes over an oxygen-implanted MoS2 catalyst (O-MoS2). The HRTEM, XRD, XPS, Raman, EXAFS and NH3-TPD characterizations show the existence of (MoOx)-O-Iv structure and abundant coordinative unsaturated (CUS) Mo sites in the 2D-layer structure of O-MoS2. In the transfer hydrogenation of nitroarenes with hydrazine hydrate, the (MoOx)-O-Iv structure works as the catalytic active center. The N2H4 selectively decomposes to the active hydrogen species in polar electronic states (H delta- and He delta+), which show high chemoselectivity toward the nitro reduction over C=C, C=C, and C N groups. The O-MoS2 catalyst can be recovered in a facile manner from the reaction mixture and recycled four times without any significant loss of activity. (C) 2016 Elsevier B.V. All rights reserved.