Polymer self-assembly can prepare various shapes and sizes of pores, making it widely used. The complexity and diversity of biomolecules make them a unique class of building blocks for precise assembly. They are particularly suitable for the new generation of biomaterials integrated with life systems as they possess inherent characteristics such as accurate identification, self-organization, and adaptability. Therefore, many excellent methods developed have led to various practical results. At the same time, the development of advanced science and technology has also expanded the application scope of self-assembly of synthetic polymers. By utilizing this technology, materials with unique shapes and properties can be prepared and applied in the field of tissue engineering. Nanomaterials with transparent and conductive properties can be prepared and applied in fields such as electronic displays and smart glass. Multi-dimensional, controllable, and multi-level self-assembly between nanostructures has been achieved through quantitative control of polymer dosage and combination, chemical modification, and composite methods. Here, we list the classic applications of natural- and artificially synthesized polymer self-assembly in the fields of biomedicine and materials, introduce the cutting-edge technologies involved in these applications, and discuss in-depth the advantages, disadvantages, and future development directions of each type of polymer self-assembly.