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The ability to efficiently separate CO2 from other light gases using membrane technology has received a great deal of attention due to its importance in applications such as improving the efficiency of natural gas and reducing greenhouse gas emissions. A wide range of materials has been employed for the fabrication of membranes. This paper highlights the work carried out to develop novel advanced membranes with improved separation performance. We integrated a polymerizable and amino acid ionic liquid (AAIL) with zeolite to fabricate mixed matrix membranes (MMMs). The MMMs were prepared with (vinylbenzyl)trimethylammonium chloride [VBTMA][Cl] and (vinylbenzyl)trimethylammonium glycine [VBTMA][Gly] as the polymeric support with 5 wt% zeolite particles, and varying concentrations of 1-butyl-3-methylimidazolium glycine, [BMIM][Gly] (5–20 wt%) blended together. The membranes were fabricated through photopolymerization. The extent of polymerization was confirmed using FTIR. FESEM confirmed the membranes formed are dense in structure. The thermal properties of the membranes were measured using TGA and DSC. CO2 and CH4 permeation was studied at room temperature and with a feed side pressure of 2 bar. [VBTMA][Gly]-based membranes recorded higher CO2 permeability and CO2/CH4 selectivity compared to [VBTMA][Cl]-based membranes due to the facilitated transport of CO2. The best performing membrane Gly-Gly-20 recorded permeance of 4.17 GPU and ideal selectivity of 5.49.