We demonstrate the advantageous use of an ultraviolet-assisted curing for the preparation of polycrystalline zeolites. The ultraviolet-assisted curing effectively hydrophobizes the porous structure of a spin-on Silicalite-1 film by means of silanol condensation and grafting of desorbing organic template fragments. Moreover, it enhances the packing of the grains, so the intergrain voids are substantially shrunk and the mechanical properties improved.