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Abstract Gas-responsive polymers have recently attracted considerable interest as unconventional smart materials that provide a new path toward the utilization of specific gases including CO2. Herein, we report gas-responsive elastomers that enhance mechanical properties, such as modulus, strength, stretchability, and toughness with CO2 gas. Various types of amine groups are introduced into polydimethylsiloxane elastomers to achieve the gas-induced mechanical reinforcement. In these elastomers, the amines form ionic crosslinks with CO2 gas that mechanically strengthen the materials. Furthermore, nanodomains formed via microphase separation of the ionic components behave similarly to viscoelastic nanofillers that dissipate a large amount of energy during deformation, thereby remarkably toughening the elastomers. Surprisingly, the fracture energy of the elastomer with diamine increases ~35 times in CO2 gas compared with that in N2 gas. Furthermore, the elastomers sensitively respond even to CO2 gas concentrations as low as 10 % and are remarkably toughened. Our design concept is widely applicable to the CO2 reinforcement of other polymers, such as polyethylene.