Zeolites and molecular sieves are synthesized using organic structure-directing agents (SDAs) that have the potential to be degraded into fragments within the pore space so that they can be readily extracted at mild conditions. The zeolites and molecular sieves, VPI-8, ZSM-12, and ZSM-5, are synthesized using the ketal-containing SDA, 8,8-dimethyl-1,4-dioxa-8-azoniaspiro[4,5]decane (SDA-1). As expected, solids with unidimensional pore systems (VPI-8, ZSM-12) are much more difficult to process by this methodology than solids containing multidimensional pore systems (ZSM-5). Pore-filling agents (PFAs) such as isobutylamine and cyclopentylamine are used together with the ketal-containing SDA-1 to prepare ZSM-5. Extraction of the PFA is shown to be feasible, and its removal provides space for components to enter the zeolite micropores where they react with and cleave SDA-1. Removal of the cleavage fragments from SDA-1 gives ZSM-5 that has the appropriate pore volume, framework aluminum (measured by Al-27 NMR), and catalytic behavior. Reasons for desiring this new type of zeolite synthesis method are enumerated.