A series of catalysts were synthesized by incorporating Mo and W active phases promoted with Co, Ni, or Fe, on a mesoporous delaminated vermiculite. The resulting solids were characterized by X-ray diffraction, temperature-programmed reduction with H2 (TPR-H2), temperature-programmed desorption of ammonia (TPD-NH3), N2 adsorption/desorption isotherms, and transmission electron microscopy. The catalytic performance of the materials was evaluated in the hydrocracking reaction of Athabasca Bitumen. The results indicate that the delaminated vermiculite is a promising material as catalytic support with acidity properties and texture which are appropriate for the synthesis of successful catalysts in the hydrocracking reaction of heavy crudes. The redox properties of the catalysts are important in the catalytic performance, the catalysts with the Mo active phase promoted with Ni and Fe being those that exhibit better activity in the hydrocracking of Bitumen.