Visualization of Solvent‐Induced Structure Evolution in Cyclodextrin Polyrotaxane Gels

Cyclodextrin (CD)-based polyrotaxanes (PR) are widely used to construct high-mechanical-performance materials because of the high degree of conformational freedom. However, strong hydrogen bonds between CDs greatly limit the application of CD-PR in the preparation of ductile neutral hydrogels. In this work, spiropyrane (SP) into α-CD-based PR is introduced to "visualize" the segment motion of the network in neutral water. The aggregation-induced cohesion and critical factors for the force transmission are disclosed. This system offers a new approach for the fundamental research for the complicated topologically cross-linked structures, which is important for the design of CD-PR-based biocompatible soft materials.