Over the last 15 years there has been considerable and increasing interest in the synthesis of zeolite films for separation-membrane and membrane-reactor applications. [1] Preparation of zeolite films on nonporous substrates for chemical sensor applications has also been reported.[2] These efforts were mostly motivated by the desire to take advantage of zeolites inherent molecular-sieve characteristics. But recently, other interesting applications, which do not rely on the molecular-sieve effect, have been demonstrated, [3] such as corrosion-resistant coatings, [4] films with low dielectric constants, [5] hydrophilic and antimicrobial coatings, [6] and heat pumps. [7] These new applications promise to offer even more exciting opportunities.High-silica zeolite (HSZ) MFI coatings for aluminum alloys, stainless steels, and carbon steels show excellent corrosion resistance, strong adhesion to the substrates, and extraordinary thermal and mechanical properties.[4] All these properties, plus the fact that zeolites are nontoxic, suggest that zeolite coatings have the potential to become an environmentally friendly alternative for the most commonly used, toxic, carcinogenic, and strictly regulated chromate conversion coating. However, zeolite coatings are normally synthesized on the substrates in water (hydrothermal synthesis) or other traditional organic solvents (solvothermal synthesis) in sealed reactors. The current hydrothermal deposition process for HSZ-MFI coatings is considered inconvenient by the surface-finishing industry, because it involves the autogenous pressure (about 9 atm at 175 8C for HSZ-MFI coating synthesis), while the chromate conversion coating can be deposited at ambient pressure.Recently, a new ionothermal method was introduced to the synthesis of zeolite powders under ambient pressure in open vessels, [8][9][10] in which ionic liquids were used instead of water or organic solvents. An ionic liquid is a substance that consists only of ions and has a melting temperature below 100 8C. Ionic liquids have been recognized as environmentally benign solvents and "designer solvents", because they have negligible vapor pressure, high chemical and thermal stability, high ionic conductivity, wide electrochemical potential windows, can act as catalysts, are nonflammable, and have tunable physicochemical properties by suitable choice of cations and anions. [11,12] These remarkable properties enable ionic liquids to be widely used in organic, inorganic, polymer, and biocatalytic synthesis. [12] AEL powder is the first example of a zeolite successfully synthesized ionothermally.[8] It was prepared under ambient pressure in a convection oven in 68 h at 150 8C using 1-methyl-3-ethylimidazolium bromide ([emim]Br) as both solvent and template. This method is also successful with microwave heating, in which case only one hour was needed for the crystallization owing to the rapid microwave absorption of ionic liquids.[9]Herein, we present the first ionothermal synthesis of zeolite films by in situ crystallization o...