Reducing carbon dioxide (CO2) is an area of great interest in current international efforts geared toward lowering emissions and combating global warming. In this work, amino-silica composite membranes were prepared and used to capture carbon dioxide. The surface of silica particles was chemically modified with amine to efficiently capture carbon dioxide. The phase separation technique was used to prepare the membranes from a composite containing polyvinylidene-fluoride-hexafluoropropylene (PVDF-HFP), amino-silica particles, acetone and water. SEM images revealed that the membranes composed of multilayers of porous polymer uniformly impregnated with silica particles. Both XRD and FTIR results have validated the perfect integration of silica particles within the polymeric network. The mechanical properties of the membrane are improved by the presence of silica particles as proved by the high tensile strength value (1.5 N/cm2) obtained for the PVDF-HFP/SiO2 membrane compared to 0.9 N/cm2 obtained for bare PVDF-HFP membrane. Also, we succeeded in recording SEM images to show that the plastic deformation of the film is associated with the formation of macro-holes. To the best of our knowledge this is the first time for such results to be monitored with SEM to observe the macroscopic evolution of the structure. Additionally, the surface area was significantly increased from 3.8 m2/g for bare PVDF-HFP membrane to 116.4 m2/g for PVDF-HFP impregnated with silica particles. Moreover, the CO2 separation efficiency depends on both surface area and the quantity of amino-SiO2 added to the membrane. The addition of amino-silica particles leads to a significant uptake of carbon dioxide compared to non-modified polymer membrane. The results obtained indicated that combing the phase separation with amino silica particles provided a cost-effective route to scaling up the synthesis of membranes that were mechanically stable and highly efficient at CO2 capture.