Immobilization and reuse of CO2 are urgent tasks for sustaining the global environment. Here it is demonstrated that CO2 can be immobilized by reaction with H2O at room temperature (RT) in the specific sub‐nm space of 1D uneven‐structured C60 polymer (1D polymer) film, even though the reaction does not occur at RT in the gas phase (activation energy: 2 eV). First‐principles calculations reveal that the CO2 molecule is stacked as a bridge between the concave portions of adjacent 1D polymer frameworks via locally induced Coulomb interactions. Such induced charge polarization activates CO2 both by weakening its double‐bonds and by lowering its lowest unoccupied molecular orbital energy due to the bending motion. In addition, the flexible π orbitals of the 1D polymer provide the optimal Coulomb field to stabilize the transition state of the CO2 + H2O reaction remarkably. These factors work together to make the reaction possible at RT.