Switching Multivalent DNA Complexation using Metal‐Controlled Cationic Supramolecular Self‐Assemblies

We provide a proof‐of‐principle that coordination chemistry drives the in situ self‐assembly of an inactive ligand into a multivalent cluster capable of effectively complexing DNA. We show that metal coordination and scavenging can be used to switch the multivalency of the system. Thus, controlled DNA complexation and decomplexation could be achieved. On demand: Metal coordination and scavenging processes enable the switching of multivalent DNA complexation through the controlled self‐assembly of cationic grid complexes.