With its extraordinary properties as the strongest and stiffest material ever measured and the best-known electrical conductor, graphene could have promising applications in many fields, especially in the area of nanocomposites. However, processing graphene-based nanocomposites is very difficult. So far, graphene-based nanocomposites exhibit rather poor properties. Nacre, the gold standard for biomimicry, provides an excellent example and guidelines for assembling two-dimensional nanosheets into high performance nanocomposites. The inspiration from nacre overcomes the bottleneck of traditional approaches for constructing nanocomposites, such as poor dispersion, low loading, and weak interface interactions. This tutorial review summarizes recent research on graphene-based artificial nacre nanocomposites and focuses on the design of interface interactions and synergistic effects for constructing high performance nanocomposites. This tutorial review also focuses on a perspective of the dynamic area of graphene-based nanocomposites, commenting on whether the concept is viable and practical, on what has been achieved to date, and most importantly, what is likely to be achieved in the future.

Bioinspired ternary rGO–MMT–PVA nanocomposites were successfully fabricated via the synergistic toughening effect from building blocks of GO and MMT nanosheets.

Ultrastrong bioinspired graphene-based fibers are designed and prepared via synergistic toughening of ionic and covalent bonding. The tensile strength reaches up to 842.6 MPa and is superior to all other reported graphene-based fibers. In addition, its electrical conductivity is as high as 292.4 S cm(-1). This bioinspired synergistic toughening strategy supplies new insight toward the construction of integrated high-performance graphene-based fibers in the near future.

Natural nacre exhibits extraordinary functional and structural diversity, combining high strength and toughness. The mechanical properties of nacre are attributed to (i) a highly arranged hierarchical layered structure of inorganic minerals (95 vol %) containing a small amount only of organic materials (5 vol %), (ii) abundant synergistic interfacial interactions, and (iii) formation under ambient temperature. Herein, inspired by these three design principles originating from natural nacre, the supertough bioinspired graphene-based nanocomposite fibers (BGNFs) are prepared under room temperature via sequential interfacial interactions of ionic bonding and π-π interactions. The resultant synergistic effect leads to a super toughness of 18.7 MJ m as well as a high tensile strength of 740.1 MPa. In addition, the electrical conductivity of these supertough BGNFs is as high as 384.3 S cm. They can retain almost 80% of this conductivity even after 1000 cycles of loading-unloading testing, which makes these BGNFs promising candidates for application in flexible and stable electrical devices, such as strain sensors and actuators.

Graphene-based fibers synthesized under ambient temperature have not achieved excellent mechanical properties of high toughness or tensile strength compared with those synthesized by hydrothermal strategy or graphitization and annealing treatment. Inspired by the relationship between organic/inorganic hierarchical structure, interfacial interactions, and moderate growth temperature of natural nacre, we fabricate an ultratough graphene fiber via sequential toughening of hydrogen and ionic bonding through a wet-spinning method under ambient temperature. A slight amount of chitosan is introduced to form hydrogen bonding with graphene oxide nanosheets, and the ionic bonding is formed between graphene oxide nanosheets and divalent calcium ions. The optimized sequential toughening of hydrogen and ionic bonding results in an ultratough graphene fiber with toughness of 26.3 MJ/m 3 and ultimate tensile strength of 743.6 MPa. Meanwhile, the electrical conductivity of the resultant graphene fiber is as high as 179.0 S/cm. This kind of multifunctional graphene fiber shows promising applications in photovoltaic wires, flexible supercapacitor electrodes, wearable electronic textiles, fiber motors, etc. Furthermore, the strategy of sequential toughening of hydrogen and ionic bonding interactions also offers an avenue for constructing high-performance graphene-based fibers in the near future.