self-healing polymers based on hydrogen bond [7,8] and metal-ligand coordination [9] have also been reported.Considering the long-term usage of self-healing polymers, high-humidity conditions or even underwater conditions cannot be avoided. Therefore, it is now recognized that the stabilities of self-healing polymer underwater have become necessary, not mentioning the huge importance in the areas of biological and environmental fields. [13,14] However, most reversible self-healing polymers are not stable under humid conditions owing to the limitations of their reversible bonds for self-healing process. Currently reported reversible self-healing polymers are mostly based on dynamic bonds including hydrogen bond, metal-ligand coordination, ionic interaction, etc. Majorities of these dynamic bonds are not stable in water. Water molecules can play multiple roles: donor and acceptor of hydrogen bonds, ligand, polar solvent, etc. It means the dynamic bonds will be disturbed in many ways: water molecules will saturate the hydrogen bonds, coordinate with the metal cation, as well as solvate the ions, and thus significantly lower the bonding constants of these bonds. The self-healing materials will then swell and lose their self-healing capability.Previously reported underwater dynamic bonds are mainly of two types: i) boronic acid derivatives that contain boronic-ester or boroxine bonds; [15][16][17][18][19][20] ii) hydrogen bonds between catechol groups, which are inspired by nature. [19][20][21][22][23][24][25][26] However, they both have many limitations. The boronic acid derivatives suffer from severe hydrolysis and they are very unstable underwater. The nature-inspired catechol groups can bond well with each other and keep the adhesion underwater. However, the hydrogen bonds between catechol are very sensitive to pH conditions, which strongly restrict their practical applications. Recently, Bao and co-workers had a breakthrough of using specially designed hydrogen bonding directly underwater self-healing polymers, but swelling is still a long-term concern due to the nature of water molecules. [27] The key question is, how can we design and develop a robust, reversible bond underwater, and how can we introduce the bond into self-healing polymers.Herein, we utilized a brand-new approach of polymer design and successfully developed a transparent elastomer that can autonomously self-heal under all types of water conditions. The elastomer has similar mechanical properties like conventional Polymer materials that are able to self-heal in humid conditions or even in water are highly desirable for their industrial applications. However, the development of underwater self-healing polymer materials is very challenging since water molecules can readily disturb traditional noncovalent bonds, such as saturate the hydrogen bonds, coordinate with the metal cation, as well as solvate the ions. Here, a new type of dipole-dipole interactions is employed as the driving force, combining with highly polar and hydrophobic fluorinated pol...