Carbon-based materials are well established as low-cost,
easily
synthesizable, and low regeneration energy adsorbents against harmful
greenhouse gases such as CO
2
. However, the development
of such materials with exceptional CO
2
uptake capacity
needs well-described research, wherein various factors influencing
CO
2
adsorption need to be investigated. Therefore, five
cost-effective carbon-based materials that have similar textural properties,
functional groups, and porous characteristics were selected. Among
these materials, biordered ultramicroporous graphitic carbon had shown
an excellent CO
2
capture capacity of 7.81 mmol/g at 273
K /1 bar with an excellent CO
2
vs N
2
selectivity
of 15 owing to its ultramicroporous nature and unique biordered graphitic
morphology. On the other hand, reduced graphene revealed a remarkable
CO
2
vs N
2
selectivity of 57 with a CO
2
uptake of 2.36 mmol/g at 273 K/1 bar. In order to understand the
high CO
2
capture capacity, important properties derived
from adsorption/desorption, Raman spectroscopy, and X-ray photoelectron
spectroscopy were correlated with CO
2
adsorption. This
study revealed that an increase in ultramicropore volume and sp
2
carbon (graphitic) content of nanomaterials could enhance
CO
2
capture significantly. FTIR studies revealed the importance
of oxygen functionalities in improving CO
2
vs N
2
selectivity in reduced graphene due to higher quadruple–dipole
interactions between CO
2
and oxygen functionalization of
the material. Apart from high CO
2
adsorption capacity,
biordered ultramicroporous graphitic carbon also offered low regeneration
energy and excellent pressure swing regeneration ability for five
consecutive cycles.