Abstract: Phillipsite zeolite particles and membranes were successfully synthesized at different operational and environmental conditions. Using an L9 orthogonal array of the Taguchi method, effects of experimental condition—synthesis temperature (130–150 °C), synthesis time (2–3 days), number of synthesized layers (1–3), and seeding suspension percentage—for membrane preparation with respect to CO2/CH4 ideal selectivity were investigated. The results showed that the ideal selectivity was improved up to 4.20 from 1.15 by increasing the number of synthesized layers, synthesis temperature, and seed solution concentration and by decreasing synthesis time. Moreover, the best synthesis conditions were defined based on the Taguchi method results and the membrane was synthesized with the highest ideal selectivity which was around 4.40. In addition, it was shown that T zeolite is formed beside PHI zeolite at low temperature even with long synthesis time.