Membranes that both have high gas permeability and selectivity is still challenging. Aiming to efficiently separate and purify ammonia-containing gases, this work constructed a novel ternary mixed matrix membranes (MMMs) by introducing functionalized ionic liquid ([Bim][NTf2]) and Cu-based metal organic framework (CuBTC). It was proved that the interaction networks consisted of hydrogen bonding and electrostatic interactions are formed in the IL-based MMMs, leading to the improved compatibility, decreased crystallinity and amorphous morphology. The ammonia separation performance was evaluated through pure gases and mixed gases. The PCu3-IL100 MMM exhibits great ideal selectivities (αNH3/N2 = 530.1 and αNH3/H2 = 94.2) and optimal NH3 permeability up to 3680.0 barrer, which is 260% and 129% higher than the pristine Pebax membrane and the PCu3 MMM, respectively. The improving NH3 separation performance is attributed to the synergistic interaction of hydrogen bonding and Lewis acid-base between IL-based MMMs and NH3 molecules, significantly increasing NH3 solubility coefficient and solubility selectivity. The IL-based MMMs also show exceptional NH3 mixed separation performance and long-term operation stability.