AbstractThe manufacture of tailored carbon‐based adsorbent structures with exceptionally low‐pressure drops and improved kinetics using stereolithographic 3D printing is presented. Adsorbent structures are printed from commercial resins with square, circular, and hexagonal cross‐sectional microchannels. These structures can reduce energy use by 50–95% compared to conventional carbon‐packed beds. The activated 3D printed carbon achieves Brunauer–Emmett–Teller surface areas over 1000 m² g⁻¹ and shows outstanding butane adsorption capacities, over twice the capacity of a commercial carbon and a comparable capacity to phenolic‐based carbons. The structures also show excellent uptakes of cyclohexane, up to 0.62 g g⁻¹ in a saturated feed. The introduction of complex axial geometries including spirals and chevrons enable superior adsorption kinetics and premature breakthrough of contaminants at high gas flow rates. These results demonstrate the success of intelligent manufacturing of low‐pressure drop, high‐capacity micro‐structured adsorbents, allowing for the development of gas separation technologies for applications such as greenhouse gas removal and respiratory protection.