This work presents the encapsulation of two amino acid-based ionic liquids (AAILs), 1-Ethyl-3-methylimidazolium glycine [Emim][Gly], and 1-Ethyl-3-methylimidazolium alanine [Emim][Ala], into an highly porous metal organic framework, MOF-177, to create a state-of-the-art composite for post-combustion CO2 capture. The AAILs@MOF-177 composite sorbents were synthesized at varying loadings of AAILs. These composite sorbents were then evaluated and examined for their thermal and structural integrity, CO2 capture capability, CO2/N2 selectivity, and heat of adsorption. Thermogravimetric analysis of the composites demonstrated that the encapsulation was successful, and the slow degradation of the composites suggested that AAILs and MOF-177 interacted with each other to some extent. Both the surface area and the pore volume of the composites experienced a dramatic decrease as a direct result of the encapsulation of the AAILs. The findings of the XRD analysis also showed that an increase in the loading of AAILs greater than a particular limit produced a degradation in the structural integrity of the parent support. At pressures below 1 bar (post-combustion conditions), the AAILs encapsulated composites outperformed the pure MOF177 in terms of CO2 uptake and selectivity. The maximum CO2 uptake was found to be at 20 wt.% loading for both [Emim][Gly]@MOF-177 and [Emim][Ala]@MOF-177 at 0.2 bar, 303 K, and the uptake values were about three times higher than MOF-177. In addition, the CO2/N2 selectivity of 20-[Emim][Gly]@MOF-177 and 20-[Emim][Ala]@MOF-177 increased from 5 (pristine MOF-177) to 13 and 11, respectively. However, it was discovered that the ideal amount of AAILs was 20 wt.%, and after that, increasing the loading any further, even to 30%, did not increase the CO2 uptake. The results of this study shed light on the stability of AAILs@MOF-177 composites, as well as their overall performance in capturing CO2 and CO2/N2 selectivity under post-combustion CO2 capture conditions.