Using inspiration derived from studying naturally occurring minerals, a series of framework beryllosilicates have been synthesized under hydrothermal conditions. These include two new zeolite topologies, a unique layered beryllosilicate, and beryllosilicate analogues of numerous aluminosilicate zeolites. Materials with the structure of the rare zeolite mineral nabesite have been synthesized for the first time, including both sodium and potassium derivatives. The structural chemistry of these beryllosilicates frameworks is discussed with reference to the networks of linked tetrahedra, which include the first instance of pentagonal, two-dimensional Cairo-tiling of silicate tetrahedra in one of the new zeolite topologies, their porosity, and their thermal stability.