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Herein, ultralong α‐CaSO4·0.5H2O whiskers with an average length above 500 µm and aspect ratios of 200–500 are hydrothermally produced employing trace amount (0.06 mg L−1) of cationic polyacrylamide (CPAM) as the morphology modifier. The hydrothermal formation mechanisms of α‐CaSO4·0.5H2O involving the initial nucleation of bassanite nanocrystals/nanorods and their subsequent self‐assembly into long...