The layer-by-layer (LbL) assembly technique is a simple, inexpensive, and versatile process for the assembly of highly ordered multilayer film of hybrid polymer-nanoparticles structures. However, each cycle in the traditional lbl dipping method takes about 5 to 20 minutes to be produced, since it depends on times of diffusion and adsorption of polyelectrolytes molecules and colloidal particles in a substrate. Therefore, macroscopic nanocomposites films with micron-size thickness can take days to be prepared. In order to speed up the lbl assembly we have produced multilayered nanolaminates by the spin-spray lbl technique. In this method, the molecular layers are formed by spraying the polyelectrolytes or nanoparticles in a high speed rotating substrate, in such a way that the adsorption of these specimens on the substrate is almost instantaneous. Consequently, we have deposited layers with cycle time as short as 1 minute by this technique, which is about 20 times shorter than in traditional lbl dipping method. In this work, utilizing spin-spray lbl technique, we have assembled nanocomposites films containing layered double hydroxide (LDH) platelets. We have achieved freestanding films with a thickness of about 10 microns comprising 1000 bi-layers produced within a time of about 8 hours. Even though these films have a high inorganic content (about 30 wt%) they are transparent. Electronic microscopy analyses unveil a structure with high spatial organization and orientation of layered inorganic nanoparticles and low concentration of aggregates of LDH.