The need to expand further the range of mesomorphic organization, develop original materials where different functionalities can be added (i.e. multifunctional), and to design “multitask materials” with tunable properties are particularly interesting and crucial challenges for potential uses in future technologies. On the one hand, we focused on the design and synthesis of multifunctional materials (liquid crystalline, dendritic, photoresponisve) which are suitable for making thin films where photoinduced optical anisotropy and surface relief gratings can be generated. The mesomorphic behaviour of these dendrimers was investigated and also their optical properties. On the other hand, we grafted structurally related protodendritic mesogenic ligands to monodisperse gold nanoparticles to elaborate liquid crystalline hybrids in order to self-organize NPs in periodic arrays. A set of dendronized gold nanohybrids was synthesized to carry out this study.