In this chapter, we present a brief introduction of the synthesis and properties of the CO 2-responsive polymers with different CO 2-responsive functional groups (tertiary amine, amidine, guanidine, imidazole, and carboxylic acid). Then we focus on the self-assembly behaviors of CO 2-responsive polymers and the size, shape, and morphology transformation behaviors of their assemblies as triggered by CO 2. Finally, we provide a review of selected recent studies demonstrating the potential applications of CO 2-responsive polymer assemblies in the field of controllable encapsulation and release, CO 2-induced gelation, and CO 2-switchable surfactants.