ABSTRACT Nacre, a biologically derived composite, is known for its hierarchical brick‐and‐mortar arrangement of inorganic platelets in an organic matrix, which contributes to its remarkable properties. Inspired by nacre's exceptional strength and toughness, this study investigates the mechanical and thermal properties of solution‐processed composite films. These films are fabricated with varying proportions of graphene oxide (GO) and biomass gasification–derived carbon nanomaterials (BGCNM) in a polyvinyl alcohol (PVA) matrix. To evaluate the effect of BGCNMs on the composite films, a range of analytical techniques were used, including X‐ray diffraction (XRD), Fourier‐transform infrared (FTIR) spectroscopy, and Raman spectroscopy. Mechanical and thermal properties were assessed through tensile testing, Vickers hardness testing, and thermogravimetric analysis (TGA). The results show that incorporating BGCNMs improves the composite films' properties. Specifically, both the tensile strength and elongation of the films increased with higher amounts of BGCNMs. Furthermore, Vickers hardness measurements demonstrated that the films became up to 8 times harder with BGCNM incorporation, and the thermal stability of the composite films was also enhanced.