An MFI zeolite nanosheet-pillared montmorillonite clay (MPC) composite material has been synthesized under hydrothermal conditions by a recrystallization method. The hierarchical porous material possesses uniform micropores in the crystalline zeolite pillars and uniform mesopores between the zeolite pillars in the clay interlayer galleries. The MPC material exhibited higher activity and better selectivity in hydrocracking of residual oil than either MFI or the montmorillonite clay pillared with silica (SPC) or the mixture of both.