Abstract:CO2-responsive polymers are a class of novel and smart macromolecules developed in recent years. They can be defined as specific polymer systems that can respond to CO2 stimulus and result in reversible structural changes. Since one only introduces CO2 gas into the polymer system, it can effectively avoid the byproduct accumulation of traditional stimulation modes such as acids, bases, redox agents, ions, and enzymes. Utilizing CO2-responsiveness these polymers can be applied in a broad spectrum of fields. This review aims to summarize the synthesis, characterization, self-assembly, and applications of these new CO2-responsive polymer systems, and propose the potential perspectives of these smart macromolecules.