In this study, we have constructed an automatic spray machine for producing polyelectrolyte multilayer films containing various functional materials on wide substrates via the layer-by-layer (LbL) assembly technique. The proposed machine exhibits advantages in terms of automation, process speed, and versatility. Furthermore, it has several features that allow a fully automated spraying operation, such as various two-dimensional spraying paths, control of the flow rate and operating speed, air-assist fan-shaped twin-fluid nozzles, and an optical display. The robot uniformly sprays aqueous mixtures containing complementary (e.g., oppositely charged, capable of hydrogen bonding, or capable of covalent bonding) species onto a large-area substrate. Between each deposition of opposite species, samples are spray-rinsed with deionized water and blow-dried with air. The spraying, rinsing, and drying areas and times are adjustable by a computer program. Twenty-bilayer flame-retardant thin films were prepared in order to compare the performance of the spray-assisted LbL assembly with a sample produced by conventional dipping. The spray-coated film exhibited a reduction of afterglow time in vertical flame tests, indicating that the spray-LbL technique is a simple method to produce functional thin film coatings.