We present the design and verification of a desktop system for the automated production of nanostructured thin films via spin-assisted layer-by-layer (spin-LBL) assembly. The utility of this system is demonstrated by fabricating polyvinyl alcohol/clay nanocomposites. Ellipsometry measurements demonstrate that the automated spin-LBL method creates composites with bilayer thickness and growth rate comparable to traditional dip-LBL; however, the cycle time of the spin-LBL method is an order of magnitude faster. Small angle X-ray scattering analysis shows that the clay platelets in spin-LBL nanocomposites are more highly aligned than in dip-LBL composites. This method can significantly increase the throughput of laboratory-scale LBL discovery and processing, can enable testing of functional properties of LBL nanocomposites over wafer-scale areas, and can be scaled to larger substrates for commercial production.