Reversible Formation of a Light‐Responsive Catalyst by Utilizing Intermolecular Cooperative Effects

A photoresponsive system where structure formation is coupled to catalytic activity is presented. The observed catalytic activity is reliant on intermolecular cooperative effects that are present when amphiphiles assemble into vesicular structures. Photoresponsive units within the amphiphilic pre‐catalysts allow for switching between assembled and disassembled states, thereby modulating the catalytic activity. The ability to reversibly form cooperative catalysts within a dynamic self‐assembled system represents a conceptually new tool for the design of complex artificial systems in water.