Ultrathin and robust nanocomposite membranes were fabricated by incorporating graphene oxide (GO) sheets into a silk fibroin (SF) matrix by a dynamic spin-assisted layer-by-layer assembly (dSA-LbL). We observed that in contrast to traditional SA-LbL reported earlier fast solution removal during dropping of solution on constantly spinning substrates resulted in largely unfolded biomacromolecules with enhanced surface interactions and suppressed nanofibril formation. The resulting laminated nanocomposites possess outstanding mechanical properties, significantly exceeding those previously reported for conventional LbL films with similar composition. The tensile modulus reached extremely high values of 170 GPa, which have never been reported for graphene oxide-based nanocomposites, the ultimate strength was close to 300 MPa, and the toughness was above 3.4 MJ m(-3). The failure modes observed for these membranes suggested the self-reinforcing mechanism of adjacent graphene oxide sheets with strong 2 nm thick silk interphase composed mostly from individual backbones. This interphase reinforcement leads to the effective load transfer between the graphene oxide components in reinforced laminated nanocomposite materials with excellent mechanical strength that surpasses those known today for conventional flexible laminated carbon nanocomposites from graphene oxide and biopolymer components.