An organic filler, bis-(N-α-amido-3,4-dihydroxyphenylalanine)-1,7-heptane dicarboxylate (DOPA-C7) is applied to gas separation membranes for CO2/N2 separation. The weak interaction between SBS and DOPA-C7 improves CO2/N2 selectivity, from 14.1 to 21.1 with increasing of CO2 permeability from 347.5 to 349.7 Barrer. This phenomenon is caused by the catechol group of DOPA-C7 that can work as a Lewis Base. However, the strongly interacting PEBAX/DOPA-C7 membranes show a typical trade-off behavior, a decrease in CO2 permeability and increase in CO2/N2 selectivity with the filler contents. This results demonstrate that interactions between the filler and polymeric matrix can cause negative effects on the gas separation performance. This work opens up the feasibility of using a catecholic compound in gas separation membranes.