Recently organic-inorganic perovskite hybrid materials have been developed for solar cell applications reaching record efficiencies of more than 23%. Furthermore, these materials allow to move from a fundamentally 3D structure using small organic building blocks to essentially 2D layered structures using larger organic building blocks. This opens an avenue towards a quite new class of organic-inorganic nano-composites in which the inorganic perovskite sheet acts as a template for the self-assembly of organic chromophores confined between the sheets of the inorganic layer. Thus the complexity of the organic interlayer in organic-inorganic hybrid perovskites can be increased by introducing additional secondary interactions between different organic components, e.g. pi-interactions. Potentially an organization can be obtained for the organic chromophores that resemble the order observed in a single crystal or by sterical constraints induced by the inorganic sheet to a different type of structures and potential properties. The number of inorganic sheets can easily be tuned by changing the stoichiometry of the organic small and large building blocks. In this way, a fluent transition of electro-optical properties can be achieved of the inorganic part from confined 2D structures to strongly delocalized quasi-3D structures.  We will present the concept and discuss the structures obtained so far. The use of carbazole ammonium salts in 2D hybrid perovskites leads to materials for solar cells with enhanced photoconductivity and stronger resistance toward moisture yielding solar cells with enhanced stability [1]. Also, the use of pyrene ammonium salts to synthesize 2D hybrid perovskites has been explored and initial results on the structure and optoelectronic properties will be discussed. Transitions between 1D and 2D structures were observed by specific modification of the stoichiometry of the components and said phase changes are observed also in function of temperature. In combination with the introduction of extra secondary interactions in the organic layer, a material is obtained with an exceptionally low bandgap. These systems are explored extensively toward structural, spectroscopic and optoelectronic properties. In this way, a new group of truly organic-inorganic hybrid materials is disclosed with possible new applications for thin film electronics.