Abstract: This invention is a method for rapidly and continuously immobilizing carbon dioxide contained in various industrial off-gas streams, the carbon dioxide being immobilized as dry, stable, and substantially water-insoluble particulates. Briefly, the method comprises passing the gas stream through a fixed or fluidized bed of hydrated barium hydroxide to remove and immobilize the carbon dioxide by converting the bed to barium carbonate. The method has several important advantages: it can be conducted effectively at ambient temperature; it provides a very rapid reaction rate over a wide range of carbon dioxide concentrations; it provides high decontamination factors; and it has a high capacity for carbon dioxide.The invention is especially well suited for the removal of radioactive carbon dioxide from off-gases generated by nuclear-fuel reprocessing facilities and nuclear power plants.