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Natural gas is the cleanest fossil fuel source. However, natural gas wells typically contain considerable amounts of CO₂, with on‐site CO₂ capture necessary. Solid sorbents are advantageous over traditional amine scrubbing due to their relatively low regeneration energies and non‐corrosive nature. However, it remains a challenge to improve the sorbent's CO₂ capacity at elevated pressures relevant to natural gas purification. Here, the synthesis of porous carbons derived from a 3D hierarchical nanostructured polymer hydrogel, with simple and effective tunability over the pore size distribution is reported. The optimized surface area reaches 4196 m² g⁻¹, which is among the highest of carbon‐based materials, with abundant micro‐ and narrow mesopores (2.03 cm³ g⁻¹ with d < 4 nm). This carbon exhibits a record‐high CO₂ capacity among reported carbons at elevated pressure (i.e., 28.3 mmol g⁻¹ total …