Inorganic membranes can operate under harsh conditions. However, successful synthesis of inorganic membranes is still challenging, and its performance depends on many factors. This work reports the effect of dip‐coating duration, inlet pressure, and inlet flow rate on the flux, permeability, and selectivity of silica membranes. A silica membrane was prepared by the deposition of silica sol onto porous alumina support. The permeability test was conducted at 100 °C using a single gas of CO2 and CH4. The highest flux was observed at the maximum inlet pressure and inlet flow rate for the membrane prepared at the minimum dip‐coating duration. The neural network modeling of the membrane predicted permeabilities showed a considerably high validity regression (R ≈ 0.99) of the predicted data linked to the experimental sets. The separation factor (α) was the highest at the maximum dip‐coating duration. The synthesized silica membrane has potential for CO2/CH4 separation under harsh operating conditions. © 2019 Society of Chemical Industry and John Wiley & Sons, Ltd.