Functional
devices that use hydrogels as ionic conductors and elastomers as dielectrics
have the advantage of being soft, stretchable, transparent, and biocompatible,
making them ideal for biomedical applications. These devices are typically
fabricated by manual assembly. Techniques for the manufacturing of
soft materials have generally not looked at integrating multiple dissimilar
materials. Silane coupling agents have recently shown promise for
creating strong bonds between hydrogels and elastomers but have yet
to be used in the extrusion printing of complex devices that integrate
both hydrogels and elastomers. Here, we demonstrate the viability
of silane coupling agents in a system with the rheology and functional
composition necessary for three-dimensional (3D) extrusion printing
of hydrogel–elastomer materials, specifically polyacrylamide
(PAAm) hydrogel and poly(dimethylsiloxane) (PDMS) hydrophobic elastomer.
By introducing a charge-neutral surfactant in the PDMS and adjusting
silane concentrations in the PAAm, cast material samples demonstrate
strong adhesion. We were also able to achieve an interfacial toughness
of up to Γ = 193 ± 6.3 J/m2 for a fully extrusion
printed PAAm hydrogel-on-PDMS bilayer. This result demonstrates that
an integration strategy based on silane coupling agents makes it possible
for extrusion printing of a wide variety of hydrogel and silicone
elastomers.