Graphene
oxide (GO) has recently been highlighted as a promising
multipurpose two-dimensional material. However, free-standing graphene
oxide films suffer from poor strength and flexibility, which limits
scaling-up of production and lifetime structural robustness in applications.
Inspired by the relationship between the organic and inorganic components
of the hierarchical structure of nacre found in mollusk shells, we
have fabricated self-assembled, layered graphene-based composite films.
The organic phase of our composite is produced via environmentally friendly and economical methods based on bacterial
production of γ-poly(glutamic acid) (PGA). Composite films made
of GO, PGA, and divalent cations (Ca2+) were prepared through
a slow solvent evaporation method at ambient temperature, resulting
in a nacre-like layered structure. These biobased nanocomposite films
showed impressive mechanical properties, which resulted from a synergistic
combination of hydrogen bonding with the bacterially produced PGA
and ionic bonding with calcium ions (Ca2+). The GO/PGA/Ca2+ composite films possessed a high strength of 150 ±
51.9 MPa and a high Young’s modulus of 21.4 ± 8.7 GPa,
which represents an increase of 120% and over 70% with respect to
pure GO films. We provide rational design strategies for the production
of graphene-based films with improved mechanical performance, which
can be applied in filtration purification of wastewater in the paper,
food, beverage, pigment, and pharmaceuticals industries, as well as
for manufacturing of functional membranes and surface coatings.