Photoresponsive supramolecular polymers are well-organized assemblies containing photosensitive molecules as (co-)monomers bound together by highly oriented and reversible non-covalent interactions. They have attracted increasing interest in smart materials and systems with precisely controllable functions, such as light-driven soft actuators, photoresponsive fluorescent anti-counterfeiting, and light-triggered electronic devices. In this thesis, we studied the mechanism of photoinduced supramolecular polymerization, the difference in the assembly mechanism of supramolecular polymers in organic solvent and water, as well as molecular motor-based aggregates that show multiple stimuli response or multistate chirality and emission. Furthermore, we developed visible light-controlled stiff-stilbenes containing functional groups for late-stage modification. We hope the discovery in photoinduced supramolecular polymerization and in situ gelation of stiff-stilbene ureas pave the way for its further application as photoresponsive materials. The thermodynamic insights in supramolecular polymerization in water enrich the fundamental understanding of aqueous supramolecular polymers. Visible light-controlled stiff-stilbenes could be used for visual light-controlled supramolecular materials in the future. We expect that our studies on the multi-responsive aggregates and multistate chiral supramolecular polymers of molecular motors built the basis for developing molecular motor-driven supramolecular materials in aqueous media.