Stimuli-responsive smart polymeric materials are highly preferred for crafting advanced functional materials for both biological and non-biological applications, as their physical and chemical properties can be modulated based on environmental conditions. In this context, supramolecular polymers (SPs)&mdashone-dimensionally elongated molecular assemblies formed through noncovalent interactions&mdashare favored over conventional covalent polymers due to the inherent reversibility of noncovalent bonds, allowing them to display dynamic and responsive behaviour to external physical (heat, light) and chemical (pH, redox) stimuli. In my PhD work, I designed and synthesized stimuli-responsive supramolecular polymers using supramolecular and organic chemistry protocols. First, we developed pH-responsive supramolecular polymers of guanosine, which demonstrated thermoresponsive phase transitions similar to their covalent counterparts. Additionally, I incorporated ferrocene (Fc) and azobenzene moieties into the monomer to create dual redox- and photo-responsive supramolecular polymers. We then introduced pyridine as a metal-coordinating unit into the Fc-based monomer to develop redox-responsive metallo-supramolecular polymers, where the rotational flexibility of Fc provided directionality for efficient metal coordination. Furthermore, we synthesized an azobenzene-conjugated amino acid-based amphiphilic organogel, in which the supramolecular chirality can be controlled by the molecular chirality of the amino acid. In conclusion, we leveraged multiple chemical and physical stimuli to design smart supramolecular polymers with potential applications in diverse areas such as materials science, biotechnology, and healthcare.