Molecular Appendix Adjusted Architectural Propagations of Red‐Light Controlled Macroscopic Photoactuating Performances

Photoresponsive motions and movements have garnered tremendous research attentions over past decades. Extensive efforts have been dedicated for developing polymeric photoactuating materials, offering effective pathways to interpret photoenergy into mechanic output. UV‐light was commonly applied as the stimulating light‐source, but it posed threats on biological systems due to its phototoxicity. Developing strategies for constructing visible‐light controlled actuating systems at various supramolecular hierarchical levels remains challenging but essential to fabricate life‐like materials. Herein, we present a red‐light driven photoswitch to propagate photoswitching properties across multiple length‐scales, enabling macroscopic photoactuations. Tetra‐ ortho ‐chloroazobenzene ( AACl ) is adopted as the photoswitching cores, allowing red‐light responsiveness. Different terminal amino acids enable to adjust intermolecular distance during supramolecular assembly formations. Extra intermolecular interactions induced by phenylalanine groups ( Phe ) converts photoresponsive properties across length‐scales into reversible morphological transformations and macroscopic photoactuations. Minimized steric hindrance induced by alanine groups ( Ala ) enables supramolecular transformations together with photoactuations, while increased steric bulkiness of the isopropyl‐group of valine groups ( Val ) suppresses photoresponsive properties in the resulting supramolecular nanostructures. Red‐light responsiveness can be amplified and converted by amphiphilic tetra‐ ortho ‐chloroazobenzenes across multiple length‐scales into mechanic outputs.