Reducing greenhouse gas emissions is a critical environmental challenge, with fossil fuel consumption and deforestation as major contributors to rising CO2 levels. Membrane-based gas separation has emerged as a promising technology due to its low energy requirements, compact design, and environmental compatibility. In this study, a novel Sulfonated PolyEther Ether Ketone (SPEEK)/polyvinyl alcohol (PVA)/zinc oxide (ZnO) nanocomposite membrane was fabricated and evaluated for CO2/CH4 separation. The incorporation of ZnO nanoparticles into the SPEEK/PVA matrix was optimized to achieve uniform dispersion, enhancing both permeability and stability. Characterization by SEM, FT-IR, XRD, AFM, and TGA confirmed the successful integration of ZnO nanoparticles and demonstrated favorable structural and thermal properties. The SPEEK (70 %)/PVA (28 %)/ZnO (2 %) membrane exhibited a CO2 permeability of 40–60 Barrer with CO2 /CH₄ selectivity of 20–25, representing an effective balance of transport and selectivity. Compared to state-of-the-art membranes such as Pebax/PEG/SiO2 and Matrimid/ZIF-8, the proposed membrane delivers comparable separation performance at significantly lower production costs (≈7.5–8.5 USD/m²), highlighting its industrial scalability and economic advantage. In addition, Artificial Neural Network (ANN) modeling using a multilayer perceptron (MLP) with the Levenberg–Marquardt algorithm achieved excellent predictive accuracy (R² = 0.9999), confirming strong agreement between experimental and predicted values. This combined experimental and modeling approach demonstrates the potential of SPEEK/PVA/ZnO membranes as cost-effective, high-performance candidates for CO2 capture and natural gas purification.