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Porous organic polymers (POPs) have shown significant potential for CO₂ capture and utilization due to their high surface areas, tunable porosity, high stability, and ease of modification. Developing POPs for CO₂ capture and catalytic conversion offers a viable solution to rising CO₂ emissions. This study presents POPs composed of pyridine units, serving as dual functional materials that act as sorbents for CO₂ capture and as substrates supporting silver chalcogenolate clusters (SCCs) for catalytic CO₂ conversion. The scalable and cost-effective synthesis of these POPs enabled the design of pilot-scale breakthrough apparatus with two parallel POP sorbent beds for continuous CO₂ capture from simulated flue gas, achieving a high working capacity of 20 L_{flue gas} kg_POP⁻¹ h⁻¹ for flue gas separation. Given the practical feasibility of using POPs for CO₂ capture and the high catalytic activity of POPs loaded with SCCs in CO₂ cycloaddition, a sequential process that integrates capturing CO₂ from simulated flue gas and directly converting the captured CO₂ into oxazolidinone achieves a high space–time yield of up to 9.6 g L_POP⁻¹ day⁻¹ in continuous operation. This study provides a viable strategy for CO₂ capture and utilization using cost-effective, dual-functional porous materials.