CO2 capture and conversion have been considered as a promising solution to global warming and the storage of renewable energy. However, it is a challenge to develop a process which combines capture with conversion under mild reaction conditions and instantly respond to the intermittent power supply. In this research, plasma-based CO2 capture and splitting have been investigated by using the plasma generated in a DBD reactor packed with hydrotalcite as the solid sorbent. Results indicated that plasma is capable of desorbing CO2 from the hydrotalcite surface and this desorption starts instantly after the ignition of plasma. It was also observed that the desorption stoped when the plasma was turned off, indicating the possibility for instant control of the process. CO was produced during the plasma treatment and the average conversion of CO2 during the detectable CO production period is 41.14%. Based on the technological advantages it can provide, the discussion has been made on the potential application as syngas production within the framework of “power to gas/liquid”, and CO2 emission reduction from power plants.