Flocculation is crucial for the treatment of coal tailings in industries. In this paper, the effects of shear-induced breakage and reflocculation of the floc, settling, and dewatering of coal tailings were investigated. The results show that as shear strength increases, the settling velocity of flocculated tailings decreases. A shear rate of 200 rpm (170.6 s-1) leads to the loss of half the settling velocity. However, at high dosage cases, 200 rpm-300 rpm shear could improve the clarity of the supernatant. Small particles are flocculated preferentially, especially for particles below 10 μm. With the increase in dosage, the critical particle size for the occurrence of flocculation increases. The chaos index proposed can quantitatively reflect the degree of flocculation or reflocculation of coal tailings. At high dosage conditions, shear could enhance the dewatering performance of flocs by reconstructing the filter cake. Controlling the structure of flocs by dosage and shear strength can help obtain appropriate settling, clarifying, and dewatering performance of coal tailings.