Preparation of Robust, Room‐Temperature Self‐Healable and Recyclable Polysiloxanes Based on Hierarchical Hard Domains

The contradiction between high mechanical strength and mild healing conditions has long existed in self‐healing materials, which limits the application of self‐healing materials. The preparation of robust materials with excellent healing performance under mild conditions can effectively reduce resource waste and environmental pollution. Herein, self‐healing polysiloxane elastomer materials, APDMS‐MDI‐IPDI‐Bs, based on microphase separation strategy are reported. Through the synergistic effect of the designed urea hydrogen bond and the nitrogen‐coordinated boroxine structure, the materials can maintain high mechanical properties (maximum tensile strength up to 3.35 MPa, elongation at break up to 316%), while maintaining excellent self‐healing and recyclable ability (24 h healing efficiency at room temperature can reach 94.77 ± 3.23%), and the performance can be repeated many times without decay. APDMS‐MDI‐IPDI‐Bs also exhibit unique hydrophobicity, expanding the application scenarios of materials containing boroxine structure.