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In the face of complex water quality changes, the application of existing cationic polyacrylamide has been largely limited. In this study, a series of cationic polyacrylamides (TPADs) with excellent flocculation/dewatering performance and low dosage were synthesized through photocatalytic surface initiation using acrylamide (AM) and acryloyloxyethyl trimethylammonium chloride (DAC) as monomers and nano-TiO 2 as an initiator. Characterization using Fourier transform infrared (FTIR) spectroscopy, nuclear magnetic resonance ( 1 H NMR) spectroscopy, thermogravimetric/differential scanning calorimetry (TG/DSC) and scanning electron microscopy (SEM) was used to analyze the structural and morphological properties of TPADs. The initiation mechanism was described and the study on the properties of TPADs shows that the initiation method could obtain the copolymer with extra-high intrinsic viscosity. Furthermore, the flocculation and dewatering performance of TPADs and PADs were investigated in the micro-polluted low turbidity water flocculation test and sludge dewatering test. The application experimental results indicated that TPADs showed satisfactory turbidity removal and sludge dewatering performance by virtue of strong charge neutralization and a bridging effect. The excellent flocculation/dewatering performance was attributed to the photocatalytic surface-initiated method and the nano-TiO 2 initiator. Therefore, it is expected to open up new initiation methods in the synthesis of polymeric flocculants for a broad variety of applications., Competing Interests: There are no conflicts to declare., (This journal is © The Royal Society of Chemistry.)