Few thin films, which possess flexibility, transparency, gas shielding, thermal stability, and mechanical strength, have been reported so far, although such materials have a wide range of applications and are in demand for optoelectronic devices. Glass is superior in heat-durability, transparency, and gas-barrier properties and, therefore, normally used as a display material; however, it is inferior in flexibility, relatively heavy, and difficult to make very thin. On the other hand, plastic is superior in flexibility, formability, and transparency; however, its dimensional stability, that is, its low thermal expansion rate and gas shielding are not good enough. For example, for a typical plastic film, such as polyethylene terephthalate (PET), the glass-transition temperature and oxygen permeability are 78°C, [1] and 40 cm 3 20 lm m -2 day -1 atm -1(1 atm ≈ 101 325 Pa), [2] respectively. We have succeeded in preparing flexible thin films having all of the above-mentioned properties (in detail, oxygen permeability less than 0.1 cm 3 20 lm m -2 day -1 atm -1 , over 90 % of total visible-light transmittance, which is comparable to conventional transparent plastic films, heat-durability up to 350°C, and mechanical strength enough to be handled) by casting aqueous dispersions of a synthetic hydrophilic clay mixed with a small amount of water-soluble organic polymer. X-ray diffraction (XRD) patterns suggest a unique close-packed lamellar structure for the film, which may bring superior heat durability. The developed films are promising for use in a wide variety of optoelectronic applications. The first clay paper was shaped from bentonite by Hauser in 1938. [3,4] It was not highly transparent and not prepared with the aim of giving it a high gas-barrier property. Claybased artificial nacre had been studied, [5][6][7][8] but it was not highly transparent. Polymer-clay nanocomposite materials have been actively studied since the 1970s. [9][10][11][12][13][14][15][16][17] Most of the composites are mainly composed of plastics, and clays are only added as minor components at less than 10 wt %.[10] Although the addition improves the mechanical strength, [11] gasbarrier properties, [12] flammability reduction, [13] and dimensional stability, [14] these performances are still low. Chaiko [15,16] has developed a new and cost-effective method of producing polymer-clay nanocomposites using almost any nonpolar, commercial polymer. The surfactant-treated clays can greatly enhance a product's thermal stability, improve stiffness and strength, and increase gas-barrier performance. The oxygen-barrier properties of these nanocomposite films are over 2 000 times better than Nylon-6. Haraguchi et al. [17] prepared stretchy clay composites with high optical clarity and flexibility; however they are not highly heat durable because the clay content is limited to 30 wt %. Triantafyllidis et al. [12] prepared an epoxy-clay film composite with a high oxygen-barrier property. The film contains a higher loading of clay but is yellowish and not ...