This study investigates the carbon dioxide (CO2) sequestration potential of three different basic oxygen furnace (BOF) slags (IHE-3/15, IHE-9/17, and Riverdale) subjected to simulated landfill gas (LFG) conditions (50% CH4 and 50% CO2 v/v) in a series of batch and column experiments. Batch experiments were performed at different moisture contents (0%, 10%, 15% and 20% moisture by weight) and temperatures (7 °C, 23 °C and 54 °C) to examine the effect of moisture and temperature on the CO2 sequestration potential of the BOF slags. The column experiments were conducted under continuous humid gas flow conditions. The results from the batch experiments show that the CO2 sequestration was significantly higher in a moist state (10%, 15%, 20% moisture (w/w)) versus the dry state (0% moisture). The optimum moisture content (w/w) for CO2 sequestration was different for each BOF slag; IHE-3/15 (10%), IHE-9/17 (20%) and Riverdale (20%). The variation in ambient temperature did not show any significant effect on the CO2 sequestration capacity of the BOF slags. The CO2 sequestration capacity of IHE-3/15, IHE-9/17 and Riverdale BOF slags determined by long-term batch experiments were 105 mg/g, 80 mg/g and 67 mg/g, respectively. The IHE-3/15 slag demonstrated the highest carbonation potential and was attributed to its finer particle size and higher free lime, portlandite and larnite content. The IHE-9/17 and Riverdale slags showed significantly lower CO2 sequestration capacity in comparison to the IHE-3/15 slag. The amount of free lime, portlandite and larnite, which are considered to be the most reactive minerals during carbonation, was nearly 1.3 times less than that of the IHE-3/15 slag in the IHE-9/17 and Riverdale slags. Also, the Riverdale slag showed relatively lower CO2 sequestration in column experiment in comparison to the batch experiments, perhaps due to a high in-situ density which limited CO2 diffusion and hence the CO2 uptake. Overall, this study provides a means to analyze the suitability of the use of BOF slags in landfill covers for mitigating fugitive CO2 emissions from landfills.