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The CO₂ adsorption of a phenylene-bridged ordered mesoporous organosilica (PMO–benzene) was analyzed. The maximum capture capacity was 638.2 mg·g⁻¹ (0 °C and 34 atm). Approximately 0.43 g would be enough to reduce the amount of atmospheric CO₂ in 1 m³ to pre-industrial levels. The CO₂ adsorption data were analyzed using several isotherm models, including Langmuir, Freundlich, Sips, Toth, Dubinin–Radushkevich, and Temkin models. This study confirmed the capability of this material for use in reversible CO₂ capture with a minimal loss of capacity (around 1%) after 10 capture cycles. Various techniques were employed to characterize this material. The findings from this study can help mitigate the greenhouse effect caused by CO₂.