Capturing CO2 emitted from industrial power plants is the most efficient method for reducing global carbon emissions at present. In this work, the enhanced dynamic mechanism of CO2 capture from flue gas has been investigated through IB group transition metal functionalized carbon nanotubes (CNTs) as kinetic accelerators via the hydrate-based approach in combination with theoretical calculations and experiments. The computational results revealed that the both the hydrophilic oxygen-containing group and Cu modified CNTs not only enhanced the CO2 adsorption ability but also exhibited high selectivity towards CO2. Importantly, experiments demonstrated that the multi-walled carbon nanotubes (MWCNTs) based accelerators significantly enhanced the dynamic performance of the hydrate formation, substantially increasing gas consumption and CO2 separation efficiency. Particularly, the theoretical selected Cu@FMWCNTs mixed with THF accelerators exhibited superior kinetic indexes during the hydrate formation even under relative low pressure at 1.5 MPa with the largest CO2 separation efficiency of 76.49%, which showed Cu@FMWCNTs to be a potential kinetic accelerator for CO2 capture. This study could provide valuable findings for nanomaterial design of novel hydrate accelerators and facilitate the development of the hydrate-based technology for CO2 capture from the economic perspective of low energy consumption.