The temperature programmed synthesis technique was employed for the preparation of a new bimetallic oxycarbide-supported system, Nb-Mo-O-C/Al2O3 (Mo/Nb = 1.2;1.6;2.0). The catalysts were characterized by CO chemisorption, BET surface area measurement, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and near-edge X-ray absorption fine structure (NEXAFS). The supported bimetallic materials were tested for simultaneous hydrodenitrogenation (HDN) of quinoline and hydrodesulfurization (HDS) of dibenzothiophene. The supported bimetallic oxycarbide was found to be highly active for both HDN and HDS, demonstrating higher activities than a commercial sulfided Ni-Mo/Al2O3 when compared on the basis of active sites. NEXAFS analysis indicated that the electronic properties of the oxycarbide were modified by the interaction with the Al2O3 support.