In this paper, orthogonal experiment was designed pragmatically by five factors and five levels and then considering the content of f-CaO and MgO to determine the process parameters. Carbonation depth, content of free-CaO and MgO were quantitatively analyzed by phenolphthalein indicator, benzoic acid - ethanol standard titration solution and EDTA titration respectively. The volume stability of mortar was measured by autoclave test. The results show that the content of free-CaO of carbonated steel slag aggregate are effected, in the order from influence degree, by moisture, carbonated pressure, carbonated time, carbonated temperature and molding pressure. Their optimal parameters are 12wt.%, 0.15MPa, 8h, 60°C and 9MPa respectively. The specimens with the f-CaO content of more than 3wt.% are all spalled, and though 5wt% of MgO is existed in carbonated aggregate, volume stability mortar is unaffected.