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Membrane technology is a forward-looking approach for gas separation, while the implementation of membrane with high performance for ethylene/ethane separation still challenges the world. Herein, a multifunctional ternary deep eutectic solvent (DES)-based membrane was constructed for the cost-effective ethylene/ethane separation. The incorporation of a sweetener (Al(NO 3) 3) with the AgNO 3 /methylacetamide (NMA) mixture to form a ternary DES not only significantly promoted the ethylene/ethane selectivity but also enhanced the long-term stability of resultant membranes, which killed two birds with one stone. Various spectroscopic characterization and quantum mechanical calculations revealed that the complexing interaction between Ag+ and NMA and the complexing interaction between Al3+ and NO 3 − weakened the electrostatic interaction between Ag+ and NO 3 −, and improved the interaction energy between ethylene molecule and Ag+ carrier. By the synergy effects of two different complexing interactions, the ternary DES-based membranes exhibited high ethylene permeability, ethylene/ethane selectivity and stability, outperforming majority of the previously published data. Therefore, the membranes proved the grand potential for ethylene/ethane separation, and this work will shed light on the design of multifunctional liquid membranes for precise molecular separation. Image 1 • A multifunctional DES-based membrane was first built for C 2 H 4 /C 2 H 6 separation. • The addition of sweetener distinctly enhanced the separation selectivity. • The separation mechanism was revealed by quantum mechanical calculations. • The cost-effective membranes exhibited high performance and durable stability. [ABSTRACT FROM AUTHOR]