Recently, we have investigated the electrostatic layer-by-layer (ELBL) deposition of polycation and clay platelet ultrathin films. We have investigated the properties of these films using techniques such as ellipsometry, X-ray diffraction and atomic force microscopy (AFM). In this work, we report our results regarding the formation of this type of hybrid ultrathin films focusing on their mechanical properties as probed by nanoindentation experiments. Structural information such as film thickness, platelet coverage, surface morphology, roughness, etc., is important parameters for their potential use as coatings. We have investigated the relationship of several of these parameters with their mechanical hardness and modulus properties as a function of indentor probe depth in nanoindentation experiments. The ultrathin films have remarkable mechanical properties very different from most polymer ultrathin films.