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[Display omitted] • Cationic PAETAC & PAmPTAC were synthesized by UV-induced radical polymerization. • New polymers showed good flocculation performance of freshwater & marine microalgae. • Optimal doses of PAETAC were 50 and 4.8 mg/g for C. vulgaris & P. purpureum. • PAETAC and PAmPTAC produced stable flocs, supporting simple dewatering step. This study addresses the challenge of microalgae harvesting through the development of flocculants. Two positively charged cationic polymers including poly[2 (acryloyloxy)ethyl]trimethylammonium chloride (PAETAC) and poly(3 acrylamidopropyl)trimethylammonium chloride (PAmPTAC) were synthesized using the UV-induced radical polymerization, for harvesting both freshwater and marine microalgae. The results show that the synthesized polymers have excellent flocculation performance for both freshwater green microalgae (Chlorella vulgaris) and marine red microalgae (Porphyridium purpureum). PAETAC outperformed PAmPTAC for both Chlorella vulgaris and Porphyridium purpureum microalgae. The optimal PAETAC doses for Chlorella vulgaris and Porphyridium purpureum microalgae were 50 and 4.8 mg/g of dry biomass while the optimal PAmPTAC doses were 252 and 35 mg/g of dry biomass respectively. Additionally, the floc formation with the PAETAC was more stable than PAmPTAC, which supported the dewatering step via sieving. The superior performance can be attributed to the higher molecular weight of the PAETAC polymer when compared to the PAmPTAC polymer. In comparison to commercially available polydiallyldimethylammonium chloride (PolyDADMAC), the newly synthesised PAETAC and PAmPTAC polymers demonstrated superior flocculation efficiency at a lower dose. The findings of this study established a platform technology for designing and synthesising cationic flocculants for use in microalgae harvesting. [ABSTRACT FROM AUTHOR]