The aromatic ammonium-based layered halide compounds were obtained of bis(4-nitroanilinium)tetrachlorocadmate and bis(2-methyl-4-nitroanilinium) tetrachlorocadmate, aiming at a new type of inorganic-organic hybrid layered material. X-ray diffraction analyses of the single crystals revealed that both of the crystals take an alternate layered structure of the organic bilayer and the inorganic sheet. Cadmium ion and chloride anions form six-coordinated octahedra whose corner anions are shared with the neighboring octahedra for the crystal of bis(4-nitroanilinium)tetrachlorocadmate In the case of bis(2-methyl-4-nitroanilinium) tetrachlorocadmate crystal the inorganic portion takes distorted four-coordinated tetrahedra. The structure of the inorganic portion for the latter crystal can be considered to be caused by the distortion of a perovskite-type octahedron due to the introduction of a bulky organic molecule.