Using polyaluminium chloride (PAC) and chitosan as the main coagulant and coagulant-aid respectively, the high algae-laden water was treated by coagulation/flocculation/dissolved air flotation (C/F/DAF). When the doses of PAC and chitosan were both moderate (7.0~8.4 mg Al2O3/L of PAC and 0.6~1.0 mg/L of chitosan), the removal rates of turbidity, algae cells and TOC were all increased apparently compared with adding PAC alone. Especially, the residual aluminum concentration reduced significantly in treated water with the aid of chitosan. The structrue and strength of flocs formed by coagulation aid of chitosan were improved obviously, which proved that addition of chitosan could enhance the flocculation performance of PAC. So, in C/F/DAF process for removing algae, using chitosan as coagulant-aid can improve the flotation performance and reduce residual aluminum concentration in treated water.