In the search for new synthesis routes of zeolites, the topotactic condensation of hydrous layer silicates shows promising results in generating novel zeolite materials with distinct framework types which might have new, interesting properties as, e.g., molecular sieves or form-selective catalysts. In order to manipulate and optimise the condensation process detailed knowledge of the crystal structures is essential. The layer silicates considered here are of a special type and can be designated as high-silica hydrous layer silicates, HLSs. The structures consist of a tetrahedral layer of interconnected [SiO4]-units containing equal numbers of terminal silanol/siloxy groups on either side of the layer and of an inter-layer region where cations of low charge density (predominantly organic cations) and water molecules are located. A topotactic condensation of the layers performed at temperatures of around 500°C with simultaneous expulsion of the inter-layer constituents is able to form fully condensed, uninterrupted framework silicates. The topotactic conversion has so far been described rarely in comparison to the classical hydrothermal synthesis of zeolites. Nevertheless, several hydrous layer silicates with different layer topologies were successfully converted into zeolites of different framework types using this synthesis route: CAS (type material: EU-20, EU-20b), CDO (type material: CDS-1), FER (type material: siliceous ferrierite), MWW (type material: MCM-22), NSI (type material: NU-6(2)), RRO (type material: RUB-41), RWR (type material: RUB-24), SOD (type material: guest-free silica sodalite). Thereby, four new zeolite framework types were obtained which have not been synthesized, so far, by direct hydrothermal synthesis (CDO, NSI, RRO, RWR). This review gives an overview on the hydrous layer silicates being structurally characterized in detail, on the condensation process and on some properties of the resulting zeolite materials.