Rubbery polymeric membranes, containing amine carriers, have received much attention in CO2separation because of their easy fabrication, low cost, and excellent separation performance. The present study focuses on the versatile aspects of covalent conjugation of L-tyrosine (Tyr) onto the high molecular weight chitosan (CS) accomplished by using carbodiimide as a coupling agent for CO2/N2separation. The fabricated membrane was subjected to FTIR, XRD, TGA, AFM, FESEM, and moisture retention tests to examine the thermal and physicochemical properties. The defect-free dense layer of tyrosine-conjugated-chitosan, with active layer thickness within the range of ~600 nm, was cast and employed for mixed gas (CO2/N2) separation study in the temperature range of 25−115 °C in both dry and swollen conditions and compared to that of a neat CS membrane. An enhancement in the thermal stability and amorphousness was displayed by TGA and XRD spectra, respectively, for the prepared membranes. The fabricated membrane showed reasonably good CO2permeance of around 103 GPU and CO2/N2selectivity of 32 by maintaining a sweep/feed moisture flow rate of 0.05/0.03 mL/min, respectively, an operating temperature of 85 °C, and a feed pressure of 32 psi. The composite membrane demonstrated high permeance because of the chemical grafting compared to the bare chitosan. Additionally, the excellent moisture retention capacity of the fabricated membrane accelerates high CO2uptake by amine carriers, owing to the reversible zwitterion reaction. All the features make this membrane a potential membrane material for CO2capture.