IN the rapidly developing area of advanced zeolite materials science, the development of novel optical, electronic and magnetic materials1-5 requires the synthesis of large single crystals of a well defined habit. Crystals of a specified size and shape are needed to fabricate membranes and sensor devices6,7. Large crystals of zeolites and molecular sieves are essential for refining structures and elucidating the intrinsic absorption and diffusion properties of these materials8,9. Here we present a method for growing uniformly large and morphologically well defined single crystals of all-silica, aluminosilicate and aluminophosphate molecular sieves with dimensions in the size range 0.4-5.0 mm. Our synthetic method relies on the use of a non-aqueous solvent, a mineralizer, an optional organic templating species and reagent amounts of water. We have prepared both large-pore and small-pore materials of various framework composition and structure type.