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Porous carbons have been considered to be promising sorbents for carbon capture and sequestration. For achieving high capture capacity and CO₂/N₂ selectivity, precise control of porous structures and surface polarity is necessary. Herein we report the preparation of N-doped porous carbon via pyrolysis of microporous polyindole with KOH as the activator under N₂. Analysis results suggest that nitrogen amounts and textural properties of carbon materials could be adjusted by KOH content and pyrolysis temperature. Generally, higher V_ultramicro/V_micro ratio (up to 0.64) and higher N-doping amounts (up to 6.87 wt%) could be obtained at a relative low pyrolysis temperature and KOH content. Impressively, the porous carbons show extremely high Henry's CO₂/N₂ selectivity up to 136 at 298 K, among the highest of carbon based materials. Even measured using simulating flue gas (15% CO₂/85% N₂) at 308 K, the …