Abstract

<h2>Summary</h2> Graphene oxide (GO)-based fibers, despite their high performance, often contain large-sized GO or reduced GO (rGO), usually leading to high cost or severe environmental pollution. The crystalline-amorphous dual-phase (CADP) strategy has been proven to be an effective route to improve mechanical properties, providing a facile and feasible structural way out to fabricate high-performance fibers. Here, we report a successful preparation of a super-strong and flexible fiber by introducing a crystalline GO and amorphous ZrO<sub>2</sub> superstructure in a way that is analogous to a naturally ordered crystalline-amorphous microstructure in nacre. In virtue of a synergistic effect of the "wrinkle extension" mechanism and the "pull-out" mechanism induced by the GO@amorphous-ZrO<sub>2</sub> superstructure, the optimum GO@amorphous-ZrO<sub>2</sub>-polyvinyl alcohol fibers show excellent combination of high strength (935 MPa) and toughness (10.6 MJ m<sup>−3</sup>). The findings demonstrate that the CADP-strengthened strategy would serve as an economical and environment-friendly method to prepare GO-based fibers with high performance.

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