AbstractThis study explores fabrication and characterization of mixed matrix membranes (MMMs) for gas separation, employing a cost‐effective solution casting method. Polycarbonate (PC) and polystyrene (PS) blends are combined with graphene oxide (GO) and zirconium dioxide (ZrO2) nanofillers, with and without a deep eutectic solvent (DES) obtained through hydrogen bond exchange. Various MMMs compositions (2–20 wt%) are systematically examined using diverse characterization techniques, including differential scanning calorimetry, thermogravimetric analysis, Fourier transform infrared spectroscopy, scanning electron microscopy, porosity determination, and water contact angle analysis. The MMMs exhibit enhanced gas permeability and selectivity, surpassing conventional membrane materials. Notably, H2 gas permeability reaches outstanding levels, with the composition PC/PS‐DES‐GO/ZrO2 at 20 wt% (PBC20‐IV) demonstrating the highest value of 86.32 Barrer. This superior performance is attributed to the unique properties of ZrO2, increased sorption capacity of GO, and enhanced thermal stability due to DES. Permeability data for CO2, N2, O2, and CH4 also show significant values, aligning with the observed trends in H2 permeability. Robeson's plot for the H2/CO2 gas pair surpasses the 2008 upper bound, placing the MMMs in a novel category for gas separation membranes. The incorporation of DES‐modified nanofiller blend composites presents a promising strategy for the potential production of pure hydrogen.