A simple co-polymerization method has been employed to prepare polysilicic-zirconium (PSZr), consisting of chemical species of ZrSi24O50, ZrSiO4, and Zr5Si3. The obtained PSZr is found to be highly active as the coagulant for the purification of the raw water and humic acid wastewater. The performance of PSZr on the wastewater purification is greatly dependent upon the synthetic temperature of PSZr, and the mole ratio of Si:Zr, and the basicity of the PSZr. It shows that PSZr synthesized at the temperature of 20-25 degrees C with the mass fraction of polysilicic acid of 1.5%, the mole ratio of Si:Zr of 1:1, and a basicity of 0.25, is relatively more efficient for water purification and could achieve the UV254 (Ultraviolet wavelength less than 254 nm) and total organic carbon removals of 81.23% and 66.85% and residual turbidity of 0.86 NUT in the raw water, and the UV254 and TOC removals of 99.20% and 74.21% in simulated humic acid wastewater, respectively. These results clearly demonstrate that PSZr could be used as the coagulant for the wastewater treatments.