For the purpose of overcoming the difficulty of low removal rate of COS at low temperatures, N-doped copper oxide-supported carbon aerogels were prepared with sodium alginate as a carbon source for deep removal of COS (about 20 ppm) from natural gas. By exploring the effects of different nitrogen sources (urea, melamine and p-phenylenediamine), carbon–nitrogen ratio and carbonization temperature, p-phenylenediamine-doped copper oxide-loaded carbon aerogels (PPD-Cu/CA) with both excellent catalytic hydrolysis of COS and adsorption were prepared. The COS adsorption capacity of optimized PPD-Cu/CA was 18.6 mg·g−1 with 0.94 %Vol of water content at 40 °C, meanwhile, the COS removal efficiency at 40,000 and 70,000 mL·g−1·h−1 could reach 100 % and 94.6 %, respectively, showing excellent high space velocity resistance. Combined with characterization and experimental results, the introduction of p-phenylenediamine enriched the pore structure of the carbon carrier, increased the neutral base site, and played a positive role in the adsorption and hydrolysis of COS. This study provides a new insight into the removal of carbonyl sulfur from natural gas.