The aim of this study is to develop nanofibrous CO2 adsorbents by using of textile wastes as precursor materials. Therefore, polyacrylonitrile (PAN) and PAN/cell nanofibers were produced from acrylic textile wastes. Nanofibrous membranes were subjected to stabilization, carbonization, and chemical activation processes, respectively, to produce activated carbon nanofiber (ACnF) structures. Elemental analysis, scanning electron microscope, FTIR, and Braunauer, Emmett, and Teller analyses were carried out and CO2 adsorption performance was tested. It was observed that all samples, except PAN/cell nanofibers carbonized at 900°C, preserved their nanofibrous structure. PAN ACnFs had a lower surface area; on the other hand, they were shown to have higher carbon dioxide adsorption values compared with PAN/cell ACnFs. Reasonable adsorption capacities as high as 3.53 and 2.99 mmol/g (at 298 K at a relative pressure of 0.989) were achieved by PAN and PAN/cell ACnFs, respectively. As a result, it was investigated that sustainable ACnF‐based carbon dioxide adsorbents could be produced by the thermochemical processing of electrospun nanofibers obtained from textile wastes.