Abstract: | A supramolecular polymer was constructed from a light‐driven overcrowded alkene switch modified with two alkylated gallic acid amide pendants ( MSP‐1 ). Upon UV irradiation, stable MSP‐1 isomerized into unstable MSP‐2 , which induced the effective collapse of well‐defined cross‐linked supramolecular polymers, and the reassembly can be realized by aging at low temperature. |