Membrane technology plays a vital, applicable, and essential role in human life and industry. The high adsorption capacity of membranes can be employed for capturing air pollutants and greenhouse gases. In this work, we tried to develop a shaped industrial form of a metal-organic framework as an adsorbent material with the ability to capture CO2 in the laboratory phase. To do so, a core/shell Nylon 6,6/La-TMA MOF nanofiber composite membrane was synthesized. This organic/inorganic nanomembrane is a kind of nonwoven electrospun fiber that was prepared using the coaxial electrospinning approach. FE-SEM, surface area calculations, nitrogen adsorption/desorption, XRD grazing incidence on thin films, and histogram diagrams were applied to assess the quality of the membrane. This composite membrane as well as pure La-TMA MOF were assessed as CO2 adsorbent materials. The CO2 adsorption abilities of the core/shell Nylon 6,6/La-TMA MOF membrane and pure La-TMA MOF were as high as 0.219 and 0.277 mmol/g, respectively. As a result of preparing the nanocomposite membrane from microtubes of La-TMA MOF, the %A of the micro La-TMA MOF (% 43.060) increased to % 48.524 for Nylon 6,6/La-TMA MOF.