Graphene oxide nanosheets (GO) bring more interest in the tunable bandgap and enhanced the optical properties of nanocomposites. The developed method successfully mixed the PMMA- dissolved in dimethylformamide (DMF) with PVA dissolved in distilled water (DW) and DMF. New (PMMA-DMF)-(PVA-DW-DMF)/GO nanocomposite was successfully fabricated with various loading ratios of GO nanosheets for the first time. Several factors were applied to get fine desperation and homogeneous using the acoustic-solution casting method. Optical Microscope (OM), Fourier-transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), and UV–visible spectrophotometer were applied to investigate the structure and optical properties of the PMMA-PVA-GO nanocomposite. The OM images confirmed the fine homogenous matrix and GO distribution in the nanocomposites. FTIR spectra exhibited the most functional group of polymers and GO in the nanocomposites and strong interfacial interaction between the GO and matrix as confirmed by the shifting in the XRD patterns of the PMMA. The optical properties results of the PMMA-PVA/GO nanocomposites revealed an improvement up to 400% of the absorbance, 337% of the absorption coefficient, 51% of the refractive index, 210% of the real and 125% of the imaginary dielectric constants in terms to increase the GO concentrations, whereas the reduction in the transmittance and energy bandgap results of allowed and forbidden indirect transition were exhibited up to 9 and 16.4%, respectively. These results could grow for better and wide applications such as radiation shielding, specific optoelectronic applications, and filters ultraviolet also could use in landfilling the chemical, nuclear, and radioactive waste.