The hydrodesulfurization of thiophene was studied over unsupported nickel-neodymium bimetallic catalysts. The physical and chemical changes of bimetals were observed after calcination and presulfidation, respectively. The activity was increased with addition of neodymium to nickel catalysts and was in good correlation with the surface area of catalysts. Qualitative evidence from XRD and SEM on the role of Nd as a structural promoter were provided.