In order to gain insight into the influence of metal‐organic framework (MOF) filler and polymer on membrane performance, eight different composites are studied by combining four MOFs and two polymers. MOF materials (NH2‐MIL‐53(Al), MIL‐69(Al), MIL‐96(Al) and ZIF‐94) with various chemical functionalities, topologies, and dimensionalities of porosity were employed as fillers, while two typical polymers with different permeability‐selectivity properties (6FDA‐DAM and Pebax) were deliberately selected as matrices. The best performing MOF‐polymer composites were prepared by loading 25 wt.% of MIL‐96(Al) as filler which improved the permeability and selectivity of 6FDA‐DAM up to 32% and 10%, while for Pebax this enhancement was 25% and 18%, respectively. The observed differences in membrane performance in the separation of CO2 from N2 are explained on the basis of gas solubility, diffusivity properties and compatibility between the filler and polymer phases.