Image credit: Wiley-VCHPolymer networks possess numerous elastically defective and isolated loops that do not contribute to mechanical stiffness. Here, a supramolecular topological linking strategy is introduced to construct stiffer-yet-ductile polymer networks using supramolecular tetravalent crosslinkers. Dynamic dissociation and reassociation of crosslinks enable the formation of topologically linked loops acting as elastic springs, leading to an exceptional stiffness scaling exponent (α = 2.05). Compared with conventional systems, the materials exhibit significantly enhanced Young’s modulus, elongation at break, and work of fracture. This strategy provides a new pathway toward high-performance soft materials for load-bearing applications such as tissue implants, bioelectronic interfaces, and soft robotics.