Supporting metal–organic frameworks (MOFs) on scalable contactors such as hollow fibers provides a practical way to expedite their use in large‐scale industrial applications. Here, the development of carbon‐hollow‐fiber‐supported MOFs as adsorbent composites for gas separation processes is reported. Moreover, this work provides an effective approach for the growth of MOFs on the surface of carbon hollow fibers that are successfully produced by pyrolysis of cross‐linked Torlon hollow fibers. To fabricate MOF/carbon composites, the carbon hollow fibers are functionalized in different media to increase the surface hydroxyl groups prior to MOF growth. The MOF incorporation is performed by growing MOF‐74 and UTSA‐16 in the pores and on the outer surface of hollow fibers using dip‐coating and layer‐by‐layer techniques. The MOF/carbon composites with relatively high MOF loadings (37–38 %) and porous structures are successfully fabricated, yielding film thicknesses as high as 10–15 μm. The MOF‐74/carbon and UTSA‐16/carbon composites exhibit surface areas of 266 and 211 m2 g−1, and pore volumes of 0.28 and 0.20 cm3 g−1, respectively. As a proof‐of‐concept, the CO2 adsorption performances are evaluated and the MOF/carbon composites are shown to have relatively good CO2 adsorption capacities of 2.0 and 1.2 mmol g−1 for UTSA‐16 and MOF‐74, respectively, at room temperature and 1 bar.