Graphene-based nanocomposite films (NCFs) are in high demand due to their superior photoelectric and thermal properties, but their stability and mechanical properties form a bottleneck. Herein, a facile approach was used to prepare nacre-mimetic NCFs through the non-covalent self-assembly of graphene oxide (GO) and biocompatible proteins. Various characterization techniques were employed to characterize the as-prepared NCFs and to track the interactions between GO and proteins. The conformational changes of various proteins induced by GO determined the film-forming ability of NCFs, and the binding of bull serum albumin (BSA)/hemoglobin (HB) on GO’s surface was beneficial for improving the stability of as-prepared NCFs. Compared with the GO film without any additive, the indentation hardness and equivalent elastic modulus could be improved by 50.0% and 68.6% for GO–BSA NCF; and 100% and 87.5% for GO–HB NCF. Our strategy should be facile and effective for fabricating well-designed bio-nanocomposites for universal functional applications.
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