In this paper, we report a CO₂/N₂-switchable sol to gel transition system based on a triblock copolymer of dimethylaminoethyl methacrylate (DMAEMA) and ethylene oxide (EO), with a measured composition DMAEMA₆–EO₁₀₉–DMAEMA₆, in aqueous nanoclay dispersions. LAPONITE® is exfoliated and stabilized by Pluronic F127. The aqueous mixture exhibits a strong response to CO₂, changing from a low viscous sol to a self-healable gel. In the presence of CO₂, the PDMAEMA blocks are protonated and the positive charged triblock copolymer bridge the negative charged nanoclays, formation of a physical network. As a consequence, a sol to gel transition is observed at the macro level. Upon removal of CO₂ through bubbling with N₂, a corresponding gel to sol transition occurs due to the deconstruction of the physical network, which is a result of the departure of the deprotonated PDMAEMA blocks from the nanoclays. This sol to gel transition is fully reversible. Furthermore, the formed gel possesses excellent self-healing ability, meaning that this hydrogel is capable of autonomous healing upon damage. Thus, we believe the fundamentals of the present CO₂-responsive smart hydrogel may hold promise for a wide range of areas, such as intelligent delivery systems and smart biomaterial fields, or a potential CO₂ plugging agent for enhanced oil recovery (EOR) performed by CO₂ flooding.