Underwater adhesion plays an essential role in soft electronics
for the underwater interface. Although hydrogel-based electronics
are of great interest, because of their versatility, water molecules
prevent hydrogels from adhering to substrates, thus bottlenecking
further applications. Herein, inspired by the barnacle proteins, MXene/PHMP
hydrogels with strong repeatable underwater adhesion are developed
through the random copolymerization of 2-phenoxyethyl acrylate, 2-methoxyethyl
acrylate, and N-(2-hydroxyethyl) acrylamide with
the presence of MXene nanosheets. The hydrogels are mechanically tough
(elastic modulus of 32 kPa, fracture stress of 0.11 MPa), and 2-phenoxyethyl
acrylate (PEA) with aromatic groups endows the hydrogel with nonswelling
property and prevents water molecules from invading the adhesive interface,
rendering the hydrogels an outstanding adhesive behavior toward various
substrates (including glass, iron, polyethylene terephthalate (PET),
porcine). Besides, dynamic physical interactions allow for instant
and repeatable underwater adhesion. Furthermore, the MXene/PHMP hydrogels
exhibit a high conductivity (0.016 S/m), fast responsiveness, and
superior sensitivity as a strain sensor (gauge factor = 7.17 at 200%–500%
strain) and pressure sensor (0.63 kPa–1 at 0–70
kPa). The underwater applications of bionic hydrogel-based sensors
have been demonstrated, such as human motion, pressure sensing, and
holding objects. It is anticipated that the instant and repeatable
underwater adhesive hydrogel-based sensors extend the underwater applications
of hydrogel electronics.