This paper describes the rapid fabrication of an organic/inorganic multi-layered composite film: Parylene-poly(vinyl alcohol) (PVA)-calcium carbonate (CaCO3) composite film. CaCO3 crystals on PVA film were sandwiched between Parylene films, and thermal bonding was carried out after folding the sandwiched crystals eight times. Using this method, a millimeterthick 48-layered organic/inorganic composite film was obtained within two days, twice to twenty four times faster than conventional methods. This method enables us to develop biomimetic composite materials with superior mechanical and optical properties attributed to the multi-layered organic/inorganic structure.