The supported amorphous NiB[bentonite (Bn) catalyst was prepared by impregnation,, following the chemical reduction with KBH4 solution. The gas-phase benzene hydrogenation was used as a probe reaction to evaluate the catalytic activity. The amorphous NiB/bentonite catalyst exhibited higher activity than the Ni/bentonite catalyst; the difference is due to the formation of amorphous structure and the electronic interaction between Ni and B. Its activity and sulfur resistance were higher than those of the corresponding amorphous NiB/Al2O3 catalyst, owing to the better dispersion of active Ni and the stronger acidity over bentonite. Nd in suitable concentration could further enhance the hydrogenation activity and sulfur resistance by improving the surface area of active Ni. Such results were discussed based on various characterizations, including X-ray diffraction (XRD), inductively coupled plasma (ICP), temperature programmed desorption of hydrogen (H-2-TPD), chemisorption and poisoning of carbon disulfide (CS2).