This study focuses on improving crystalline characteristics of metal-contaminated sludge. The mineralization behavior of Cu/Al or Cu/Fe coexisting in solution is surveyed, and the characteristics of residue and suspension settling are discussed in the context of water content of residue and settling/specific filtration resistance of suspensions. Experimental data show that the hydrate of Cu 4 SO 4 (OH) 6 forms during mineralization of copper sulfate solution when hydroxide ion concentration, reaction time, and temperature are not controlled appropriately. Mineral characteristics of the residue are usually poor when the Cu 4 SO 4 (OH) 6 forms in Cu/Al or Cu/Fe solution. However, Cu 4 SO 4 (OH) 6 can be further transformed into CuO with wet oxidation or ferrite method, respectively (i.e., mineralization treatment). Water reduction of the residue is from 96.8% to 72.8% in the Cu/Al case or 95.6% to 66.6% in the Cu/Fe case, and the mineralized residue volume is only 1/10 of the hydrate sediment. This is particularly beneficial for sludge disposal.