Monolithic binder-free CO₂ adsorbents with high adsorption capacity, selectivity, adsorption-desorption kinetics, and regenerability are highly desired to both reduce the environmental impact of anthropogenic CO₂ emissions and purify valuable gases from CO₂. Herein, we report a strategy to prepare monolithic carbonaceous CO₂ adsorbents from low-cost and underutilized bioresources, which enabled the formation of a delicate anisotropic, hierarchical porous structure. With optimized material composition and processing conditions, the biobased carbon adsorbent demonstrated a CO₂ adsorption capacity of 4.49 mmol g^-1 at 298 K and 100 kPa, relatively weak adsorbent-adsorbate affinity, good CO₂/N₂ selectivity, and advantageous hydrophobicity against water vapor. Moreover, the unique anisotropic porous structure provided high stiffness and good flexibility to the adsorbent in the axial and radial directions, respectively. We confirmed that this type of carbon adsorbent could be packed in a column for dynamic CO₂ capture independent of any binders, indicating its promising future for further development toward widespread utilization.