The repair and regeneration of the body's tissue using polymeric materials remains a main focus of biomaterials research. While hydrogels and elastomers have shown biocompatibility and high extensibility, they lack the required toughness to host proliferating cells. As the need for robust polymeric scaffolds grows, new technologies must emerge to meet the stringent physical and biological needs of proliferating cells. To this end, the utilization of self-assembling motifs allows for the construction of versatile networks in which cells can grow. In this review, we discuss emerging techniques that harness the assembling capabilities of synthetic supramolecular and natural peptide motifs to construct mechanically robust elastomers and hydrogel scaffolds. In particular, we focus on how the design and structure impact their mechanical properties and interaction with the cellular environment.