Underwater adhesion is a challenging task for most synthetic
adhesives. Efforts to overcome this challenge have largely
focused on modifying natural molecules produced by marine
organisms such as mussels, sandcastle worms, barnacles, and
sea urchins.[1–4] In particular, the adhesive 3,4-dihydroxy-l-
phenylalanine (DOPA) residue found in proteins secreted by
mussels has been a popular inspiration for several synthetic
underwater adhesives.[5–7] Although such biomimetic
approaches can be powerful, synthetic materials that are
able to achieve a similar function using orthogonal methods
could be valuable alternatives. For example, most DOPA-
based adhesives require curing agents that irreversibly cross-
link the residues to the surfaces.[8, 9] Efforts to achieve
reversibility have largely been limited to the microscopic
level.[10] We thus decided to investigate whether a synthetic
system entirely unrelated to DOPA could achieve underwater
adhesion and potentially overcome limitations, such as the
lack of reversibility at the macroscopic level.