Although thin-film composite membranes have achieved great success in CO 2 separation, further improvements in the CO 2 permeance are required to reduce the size and cost of the CO 2 separation process. Herein, we report the fabrication of composite membranes with high CO 2 permeability using a laser-patterned porous membrane as the support membrane. High-aspect-ratio micropatterns with well-defined micropores on their surface were carved on microporous polymer supports by a direct laser writing process using a short-pulsed laser. By using a Galvano scanner and optimizing the laser conditions and target materials, in-plane micropatterns, such as microhole arrays, microline grating, microlattices, and out-of-plane hierarchical micropatterns, were created on porous membranes. An aqueous suspension of hydrogel microparticles doped with an amine-based mobile carrier was sprayed onto the patterned surface to form a defect-free thin separation layer. The surface area of the separation layer on the patterned support is up to 80% larger than that of flat pristine membranes, resulting in a 52% higher CO 2 permeance (1106 GPU) with a CO 2 /N 2 selectivity of 172. The laser-patterned porous membranes allow the development of inexpensive and high-performance functional membranes not only for CO 2 separation but also for other applications, such as water treatment, cell culture, micro-TAS, and membrane reactors.