We described an insect-inspired strategy for conferring reversible, high responsivity on polymer microgels to dilute-source CO2 (≤5000 ppm in gas mixtures). This is demonstrated on oligo(ethylene oxide)-based microgels that contain tertiary amines on the polymer chains with proper organic small molecular carbonates in the polymer-solvent system. Similar to the synergistic contribution of the CO2 receptor subunits in mosquitoes for CO2 response, laser light scattering and related studies indicated that the CO2-response of the microgels in terms of the volume changes works through the coordination of different functional moieties in the system, making it different from the conventional CO2-response mechanism. While this pushes the lower response threshold of CO2 concentration down to ca. 1000 ppm, this unique strategy can also satisfy the urge to achieve both effective CO2 capture and facile CO2 release, making it possible to couple the detection with the capture and utilization of indoor excess CO2.