Methanol-to-olefin (MTO) conversion on microporous silico-aluminophosphates is particularly well-suited for the application of molecular-level concepts to the development of well-defined supported catalysts. The active site of a typical MTO catalyst is a nm-size inorganic cage with an essential organic component. Opportunities for altering the selectivity of such catalysts include tailoring the organic component and modification of the cage with additional inorganic material through ship-in-a-bottle synthesis. The latter possibility has already been realized experimentally by the development of a useful and practical phosphate-modified catalyst.