In spite of the enormous level of interest in open-framework materials (materials with porous channel structures, such as zeolites), the mechanisms by which they are formed are in many cases poorly understood. As a consequence, our ability to design reaction conditions that might lead to the formation of particular crystal architectures is quite limited. This article discusses the state of the art in this area, with particular emphasis on our joint work that was recently recognized by the 2004 S miya Award from the International Union of Materials Research Societies (IUMRS) and presented at the 2004 Materials Research Society Spring Meeting/IUMRS 9th International Conference on Electronic Materials.