In recent years, self-assembly has been employed to create complex artificial molecular machines and smart materials. Various studies have been focused on the fabrication of smart functional materials where physical properties and functions emerging from large molecular self-assemblies can be controlled at will. Photoresponsive self-assembled systems are particular attractive.The aim of this thesis is to develop smart materials based on photoresponsive self-assembled systems, with a special focus on Langmuir film, liquid crystals (LC), and helicates. Chapter 1 gives a literature review on self-assembly processes and self-assembled systems which can be controlled by external stimuli. In Chapter 2, a photoresponsive Langmuir film based on amp...