Metal-organic frameworks (MOFs) are highly compatible with polymers and can be used to create mixed matrix membranes (MMMs) for gas separation. Herein, we engineered the particle size as well as the number of missing linkers in CAU-10-H MOFs via either applying the plasma treatment (CAU-10-H_Plasma) or varying the water/N,N-dimethylformamide (H 2 O/DMF) co-solvent ratios (CAU-10-H_Micro and CAU-10-H_Nano). The CAU-10-H_Nano showed the largest number of missing linkers, but the lowest adsorption uptake of CO 2 and CH 4 albeit the largest BET surface area. In contrast, both CAU-10-H_Plasma and CAU-10-H_Micro exhibited relatively high adsorption uptake of CO 2 and CH 4 . In addition, all the MMMs fabricated using 6FDA-mPDA:DABA (3:2) exhibited a good interaction between Al 2+ metal ions of CAU-10-H and carboxylic groups of 6FDA-mPDA:DABA (3:2). Importantly, the 6FDA-mPDA:DABA (3:2)/CAU-10-H_Plasma (75/25 w/w) MMM exhibited more attractive selectivities of CO 2 /CH 4 and H 2 /CH 4 (e.g., 68 and 184, respectively) compared to those of the other two MMMs under single-gas conditions. It also showed the highest CO 2 /CH 4 selectivity of 67 under equimolar CO 2 /CH 4 mixed-gas conditions. As CAU-10-H_Plasma possessed the lowest quantity of defective sites among the three CAU-10-H samples, suppressing defective sites in MOFs could be an effective approach for enhancing the CO 2 separation efficiency. • Emerging MOF, CAU-10-H, is used for preparation of MMMs. • Plasma-assisted synthesis of CAU-10-H is employed for the size and defect control. . • The CAU-10-H/6FDA-mPDA:DABA (3:2) MMM presents CO2/CH4 selectivity of of 67 with CO2 permeability of 29 Barrer under an mixed-gas permeation test. .