The silicon–aluminum–iron flocculant (PAFSi) combines the most abundant resources of waste incineration bottom ash and unpurified water, being regarded as one of the most promising approaches toward water purification. Herein, in this research, waste incineration bottom ash was employed to produce a cost-effective and highly efficient flocculant. PAFSi with a particle size of 214 nm and a zeta potential of 8.63 mV reached the optimum performance using a dosage of 2 mL/50 mL at pH from 8 to 11. The results with the copolymer exhibited the following: (1) a good flocculation efficiency over a wide pH range, (2) superior flocculation performance compared to those of polyaluminum chloride and polyferric sulfate, (3) three-dimensional branching structure of PAFSi micelles with a high aggregation degree, (4) charge neutralization and bridging as the main flocculation mechanism, and (5) recycling the floc. Thus, this work provides an attractive solution to the pressing global clean water shortage problem.