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The electrokinetic characteristics and coagulation behaviors of polyaluminum silicate chloride (PASiC) and polyaluminum chloride (PAC) were studied and compared by streaming current (SC) measurement and jar test method. The experimental results showed that the interaction between polysilicic acid characterized negative charge and hydrolyzed aluminum species result in a decrease of the charge-neutralizing ability of PAiSC, compared to PAC. The decrease has a close relationship with the basicity (B) and Al/Si molar ratio in PASiC. The less the B value and the Al/Si molar ratio, the lower the charge-neutralizing ability of PASiC is. In contrast, the preparation technique for PASiC affects the charge-neutralization of PASiC to a smaller extent. In addition, compared with PAC, PASiC may enhance aggregating efficiency and give better coagulating effects.