A bioinspired approach combining chemical bath deposition (CVD) of oxides with layer-by-layer (LBL) assembly of organic polymers has been used to prepare two different types of organic/inorganic multilayer composite films, whose morphology resembles that of naturally occurring nacre. Both process steps allow for a precise control of the layer thickness, thus enabling to tailor the architecture of the multilayer composites. The first type of composite films comprised of TiO2 layers, separated by organic interlayer composed of several oppositely charged polyelectrolytes, while the second type of composite films contained ZnO as the inorganic and poly (amino acids) as the organic component. AFM investigations revealed a granular structure of the inorganic layers which originates from the oxide particles. TEM investigation disclosed that the TiO2 particles are amorphous, while the ZnO particles are crystalline. Moreover, TEM cross-sectional analysis of the composite films confirmed the presence of inorganic layers that are well-separated by organic layers, although signatures of partial interpenetration have been observed at the interfaces. The hardness and Young's modulus of both types of composite films, as determined by nanoindentation testing, increased in comparison to the monolithic oxide films. The enhanced mechanical performance underlines the effectiveness of combining layers of different shear moduli into an alternate architecture.