Multivalency is a unique concept in nature to achieve strong interfacial reversible interactions between m‐valent ligands and n‐valent receptors of the participating binding partners (with m, n > 1) to increase the binding strength and the kinetic stability. Furthermore, multivalency plays an essential role in biological systems for recognition, adhesion, and signaling processes involving antibodies, membranes, molecules, cells, and pathogens such as viruses and bacteria [1–4]. Understanding the mode of action at the molecular level is the first priority for designing multivalent scaffolds, which can play a huge role in the fields of medicine, bio‐ and supramolecular chemistry, or materials science. The velcro fastener represents one example of these decoding and developing processes, which are necessary to achieve a marketable system. Inspired by the natural burr (Figure 9.1a), the velcro fastener (Figure 9.1b) also uses hooks and loops for reversible multivalent ligand–receptor interactions.