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In this study, a series of chitosan-based quaternary ammonium graft flocculants, namely chitosan-graft-poly(acrylamide and methacryloyl ethyl trimethyl ammonium chloride) [CTS-g-P(AM-DMC)], was successfully synthesized by plasma initiation, and the as-prepared [CTS-g-P(AM-DMC)] had both flocculation and sterilization functions. Various characterization techniques were used to study the structure and physicochemical properties of the chitosan-based flocculants. 1H nuclear magnetic resonance spectroscopy (1H NMR), Fourier transform infrared spectroscopy (FTIR), X-ray diffraction spectroscopy (XRD), and thermogravimetric analysis/differential scanning calorimetry (TG/DSC) confirmed the successful synthesis of CTS-g-P(AM-DMC). Scanning electron microscopy (SEM) analysis exhibited that CTS-g-P(AM-DMC) contained a smooth convex and porous structure with an enormous surface area. CTS-g-P(AM-DMC) was then used to flocculate the simulated wastewater of the kaolin suspension and the Salmonella suspension. Besides external factors, such as the dosage of flocculant and pH, the effect of the internal factor graft ratio was also evaluated. The experimental results showed that CTS-g-P(AM-DMC) also revealed a strong sterilization effect, aside from the excellent flocculation effect. Moreover, the sterilization mechanism was investigated through a series of conductivity measurements and the analysis of fluorescence-based cell live/dead tests. The results indicated that CTS-g-P(AM-DMC) destroyed the cell membrane of Salmonella through its grafted quaternary ammonium salt, thereby exhibiting sterilization property. [ABSTRACT FROM AUTHOR]