ABSTRACT The deployment of carbon capture, utilization, and storage (CCUS) has become a key approach to mitigating the overwhelming greenhouse effects. Porous carbon materials (PCMs) are a range of promising carbon capture candidates due to their affordability, environmental friendliness, and resistance to moisture. Numerical studies on the effect of porous structures on CO 2 uptake exist; however, these results still need to be systematically analyzed to better understand how their pore structures affect the adsorption properties. This work comprehensively summarizes pore structure construction strategies and elucidates the ideal pore structure features conducive to CO 2 adsorption, focusing on the synergistic effects of porous structures on the CO 2 adsorption capacity and CO 2 /N 2 selectivity. A specific surface area exceeding 1000 m 2 /g and a total pore volume higher than 0.5 cm 3 /g are sufficient for achieving high CO 2 adsorption capacity without necessitating excessively high values. A high proportion of narrow‐micropores (<0.7 nm) volume and a low proportion of mesopores (2–10 nm) volume are crucial for their high capacity, high selectivity, and fast diffusion. Furthermore, adsorption conditions significantly influence the adsorption capacity of narrow micropores. Precision pore engineering, condition‐responsive functional pore structure, and AI‐driven material design are recommended as research frontiers for advancing PCMs for carbon capture.