Abstract1 D multi‐walled carbon nanotube/graphene oxide nanoribbon (MWCNT@GONRs) hybrids were prepared using a chemical method as fillers for Pebax‐based mixed matrix membranes (MMMs) with excellent CO₂ separation performance. Herein, the GONRs shell provided a selective barrier and large gas adsorption area, which contributed to enhancement of gas selectivity, while MWCNTs core with smooth internal surface acted as a rapid transport channel, which improved the gas permeability. It is found that MMMs with 1 wt % loading showed the highest separation factor (80 for CO₂/N₂ and 23 for CO₂/CH₄) and high CO₂ permeability, far surpassing the upper bound line. Therefore, the synergistic effect of the MWCNTs core and GONRs shell in MWCNT@GONRs nanohybrids can effectively enhance the gas‐separation performance of MMMs at low loading. The unique microstructures, ease of synthesis and low filled loading make MWCNT@GONRs promising candidates in post‐combustion and sustainable chemistry.