Demands for high strength integrated materials have substantially increased across various kinds of industries. Inspired by the relationship of excellent integration of mechanical properties and hierarchical nano/microscale structure of the natural nacre, a simple and facile method to fabricate high strength integrated artificial nacre based on sodium carboxymethylcellulose (CMC) and borate cross-linked graphene oxide (GO) sheets has been developed. The tensile strength and toughness of cellulose-based hybrid material reached 480.5 ± 13.1 MPa and 11.8 ± 0.4 MJm by a facile in situ reduction and cross-linking reaction between CMC and GO (0.7%), which are 3.55 and 6.55 times that of natural nacre. This hybrid film exhibits better thermal stability and flame retardancy. More interestingly, the hybrid material showed good water stability compared to that in the original water-soluble CMC. This type of hybrid has great potential applications in aerospace, artificial muscle, and tissue engineering.

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In this article, a simple strategy was employed to fabricate bioinspired hybrid composite with carboxymethyl cellulose (CMC), graphene oxide, and reduced graphene oxide/alumina (rGO/Al) by a facile solution casting method. The tensile strength and toughness of rGO/Al-CMC-GO can reach 586.6 ± 12 MPa, 12.1 ± 0.44 MJm, respectively, due to the interface strengthening of alumina, which is 1.43 and 12 times higher than steel and about 4.3 and 6.7 times that of nature nacre. The artificial nacre hybrid composite is conductive due to the introduction of rGO/Al on the surface. Interestingly this structure can also be coated on the surface of cotton thread to give the thread good mechanical performance and conductivity. Additionally, the artificial nacre has better fire shielding and gas barrier properties. The oxygen permeability (OP) for 1% rGO/Al-CMC decreased from 0.0265 to 0.003 mLμm m day kpa, the water vapor permeability (WVP) decreased from 0.363 to 0.205 gmmm day kpa when the concentration increased from 1% rGO/Al to 6% rGO/Al. It is believed this work provided a simple and feasible strategy to fabricate ultrastrong and ultratough graphene-based artificial nacre multifunctional materials.