Factors affecting carbon dioxide fixation in chrysotile mining residues (CMR) under environmental conditions were studied by reproducing mineral dissolution and carbonation in laboratory columns packed with CMR particles. Carbonation is very sensitive to water saturation and watering frequency of the CMR porous media. CO2 uptake by dry residues subjected to dry CO2 flow for several days at ambient temperature was below 0.02%. However, an increase by a factor of 20 in CO2 uptake was achieved by periodic addition of small amounts of water with respect to a moistened CO2 stream over dry CMR samples. The highest MgCO3 conversion resulted in nearly 22 mg of CO2 captured per gram of residue, revealing that up to 93% of Mg remained noncarbonated because of surface obstructing processes. Magnesium leaching from CMR was hindered by two concomitant passivation phenomena limiting the residue's CO2 storage capacity. A unique cyclic voltammetry technique using oxic and anoxic aqueous solutions contacted with CMR fixed beds was implemented to assess the relative importance from CMR-borne iron electrochemical passivation and silica-deposit nonelectrochemical passivation. Passivation around the dissolving CMR particles by iron hydroxide precipitation was found to develop very rapidly in comparison to silica gel polymerization.