Multiphase‐Assembly of Siloxane Oligomers with Improved Mechanical Strength and Water‐Enhanced Healing

Abstract Healable silicone materials have great technical impact in coatings, smart actuators, and flexible electronics, however, current healable silicone materials lack mechanical tunability. Herein, we designed and synthesized a new type of healable silicone through hydrogen‐bond assisted multiphase assembly of siloxane oligomers. Besides the enhanced mechanical strength, unique water‐enhanced healing was observed in the polymer network which is due to the reversible dissociation/association of multivalent hydrogen bonds in the presence of water.