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Graphical abstract:

The human body is composed of composite structures made of water-rich hydrophilic domains and hydrophobic barriers. Combining hydrogels with elastomers results in similar synthetic biomaterials applicable to fields ranging from stretchable electronics to actuators. Here, we report a method to combine hydrogels with elastomers via a glass fiber fabric interphase. The interphase plays two roles: it enables chemically different materials to be robustly bound without chemical treatment while also dramatically improving the mechanical properties of the composite. Maximum interfacial adhesion energies of ∼1,000 N m−1between the hydrogel and fabric and ∼360 N m−1between the elastomer and fabric approach adhesion values of chemically bound soft materials. The composite tearing toughness (143 kJ m−2) vastly exceeds that of all neat components. In these materials, Young's modulus is high (∼1.2 GPa), while bending modulus is low (∼7 MPa), resulting in structures that can serve as actuators through controlled solvent exposure.