CO₂ is a major contributor to climate change, making efficient carbon capture essential for emission reduction. Membrane gas absorption (MGA) offers a cost-effective solution, with research often focusing on enhancing membrane hydrophobicity to reduce wettability. However, the potential of CO₂-philic membranes for mixed gas separation remains underexplored. This study addresses the gap by developing asymmetric wetting membranes (PVDF/EDA/GO) with a superhydrophobic side to prevent wetting and a CO₂-philic side to enhance CO₂ capture. The CO₂-philic surface was created by coating PVDF with ethylenediamine (EDA) and graphene oxide (GO). Computational analysis confirmed strong binding energy (−21.07 kcal/mol) between EDA and GO, forming a stable amine complex. The membranes displayed asymmetric wetting, with the CO₂-philic side showing a water static angle (WSA) of 49.6 ± 2.6°, and the superhydrophobic side achieved a WSA of 149.7 ± 3.3° and a water gliding angle (WGA) of 9.8 ± 1.1°. In MGA, these membranes demonstrated improved performance, with a CO₂ absorption flux of 0.0040 mol/m2s and CO₂/N2 selectivity of 6. This work highlights the promise of dual-wetting membranes for enhancing CO₂ capture in MGA systems.