▎ 摘　　要

Excellent fatigue resistance is a prerequisite for flexible energy devices to achieve high and stable performance under repeated deformation state. Inspired by the sophisticated interfacial architecture of nacre, herein a super fatigue-resistant graphene-based nanocomposite with integrated high tensile strength and toughness through poly(dopamine)-nickel ion (Ni2+) chelate architecture that mimics byssal threads is demonstrated. These kind of synergistic interfacial interactions of covalent and ionic bonding effectively suppress the crack propagation in the process of fatigue testing, resulting in superhigh fatigue life of this bioinspired graphene-based nanocomposite (BGBN). In addition, the electrical conductivity is well kept after fatigue testing. The proposed synergistic interfacial interactions could serve as a guideline for fabricating high-performance multifunctional BGBNs with promising applications in flexible energy devices, such as flexible electrodes for supercapacitors and lithium batteries, etc.