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In the current work, we presented the synthesis of N-doped hierarchically porous carbons (NDHPCs) through chemical activation of hierarchically structured precursor derived from polyvinylpyrrolidone (PVP) and magnesium acetate tetrahydrate. Magnesium acetate tetrahydrate served as the blowing agent, and its decomposition product MgO served as the in-situ formed hard template. Combined with KHCO 3 activation, the NDHPCs demonstrated a unique micro- meso -macroporous structure. Owing to the highly porous structure (1560–2545 m2/g) and enriched N-doping (1.48–6.31 wt%), the NDHPCs were investigated as potential CO 2 adsorbents in both post-combustion capture and pre-combustion capture applications. When the adsorption temperature was 25 °C, the samples showed outstanding capture performances at both 1 bar (2.97–3.88 mmol/g) and 20 bar (13.24–19.89 mmol/g). The adsorption performances were further analyzed with grand canonical Monte Carlo (GCMC) simulation. Effects of various physicochemical properties on CO 2 adsorption at different pressures were thus revealed with a combined experimental-theoretical approach. [Display omitted] • NDHPCs with unique micro- meso -macroporous structure are prepared. • The precursor is prepared through chemical blowing and in-situ hard template. • The NDHPCs demonstrate high S BET (1560–2545 m2/g) and N content (1.48–6.31 wt%). • At 25 °C and 20 bar, CO 2 uptake of the NDHPCs reaches 19.89 mmol/g. [ABSTRACT FROM AUTHOR]