Abstract: A rolling contact layer-by-layer assembly device comprises at least one roller, a cylinder substrate and a motor to rotate the cylinder substrate. The assembly device optionally includes at least one rinsing nozzle and air applicator. The rollers each provide a polyelectrolyte solution to the surface of the cylinder substrate, the polyelectrolyte solutions having an affinity for each other. Excess polyelectrolyte solution can be washed using the rinsing nozzle followed by a drying step prior to the application of the second polyelectrolyte solution. A plurality of bilayers is produced by the continuous application of polyelectrolyte solutions to form an LBL article such as a nano-composite article or film. The film is then removed from the surface of the cylinder substrate.