Zeolites and molecular sieves, a class of crystalline microporous solids with unique shape-and/or surface-selective properties, owing to the extremely uniform in shape and size of their channels and cavities, are of prime importance for industrial catalysts. If so, the development of new synthesis methods for already known zeolites is of technological relevance, as well as of scientific interest: there are many examples where the original synthesis procedure includes the use of costly organic structure-directing agents (OSDAs) and/or heteroatoms. In this work, we have synthesized zeolites with novel framework structures and compositions via a multiple inorganic cation approach in the existence of already known OSDAs. We have described the small gases (e.g., carbon dioxide, methane, and nitrogen) adsorption properties of alkali metal forms of our novel zeolites. Finally, the catalytic properties of our novel materials in Brønsted acid- and metal-catalyzed reactions. i.e., as catalyst supports as well as catalysts was investigated.