▎ 摘　　要

During the last decade, two-dimensional (2D) materials have emerged as versatile building blocks for the next generation of engineered materials. However, the intrinsically brittle behavior of 2D materials has thus far delayed their adoption in applications such as sensors and structural materials. Herein, we demonstrate a strategy for toughening graphene oxide (GO) through synergistic interfacial interactions between GO monolayers and ultrathin layers of strongly interacting poly(vinyl alcohol) (PVA). By creating GO-PVA and PVA-GO-PVA nanolaminates, we demonstrate a 2-fold increase in GO toughness, which translates into dramatic increases in energy dissipation and piercing resistance. Atomistic simulations show that this remarkable behavior arises from a polymer chain crack-bridging mechanism, resulting from a synergistic combination of interdomain reinforcements across the GO monolayer and extensive GO-polymer interfacial hydrogen-bonding interactions. The reported findings highlight the potential for achieving engineered 2D materials with superior mechanical properties by incorporating deformation and failure-resistant mechanics arising from tailored chemical interactions between constituents.