Abstract This work reports the results of a combined accelerated carbonation and wet granulation treatment applied to Basic Oxygen Furnace (BOF) steel slag with the aim of producing secondary aggregates for civil engineering applications and of storing CO2 in a solid and thermodynamically stable form. The tests were carried out in a laboratory scale granulation device equipped with a lid and CO2 feeding system. In each test, humidified slag (liquid/solid ratio of 0.12 l/kg) was treated for reaction times varying between 30 and 120 min under either atmospheric air or 100% CO2. Under both conditions, the particle size of the treatment product was observed to increase progressively with reaction time; specifically, the d50 values obtained for the products of the combined granulation and carbonation treatment increased from 0.4 mm to 4 mm after 30 min and to 10 mm after 120 min. Significant CO2 uptake values (between 120 and 144 g CO2/kg) were measured even after short reaction times for granules with diameters below 10 mm and for the coarser particle size fractions after reaction times of 90 min. The density, mineralogical composition and leaching behavior of the obtained granules were also investigated, showing that the combined granulation–carbonation process may be a promising option for BOF slag valorization, particularly in terms of decreasing the Ca hydroxide content of the slag. Another interesting finding was that the leaching behavior of the product of the combined treatment appeared to be significantly modified with respect to that of the untreated slag only for coarse uncrushed granules, an indication that the carbonation reaction occurs mainly on the outer layer of the formed granules.