A Highly Self‐Healable Elastomer Based on Heterocyclic and Cage‐Shaped Additives with Enhanced Mechanical Properties

Abstract A highly self‐healable elastomer based on heterocyclic and cage‐shaped moieties is prepared, and its self‐healing and mechanical properties are investigated. Introducing these functional moieties into a conventional elastomer significantly enhanced reversible physical interactions through intensified hydrophobic and hydrogen bonding interactions facilitated by the cage‐shaped and heterocyclic structures. The self‐healable elastomer exhibits outstanding optical properties, thermal stability, mechanical properties, and self‐healing performance compared to a conventional elastomer lacking these functional groups. These results are attributed to the formation of a unique supramolecular network driven by strong hydrophobic interactions between cage‐shaped adamantane groups and the hydrophobic regions in the matrix, along with intensified hydrogen bonding between the urethane and heterocyclic groups.