We have constructed an outer-cylinder-rotating Couette device for high-speed shear flow in laminar flow conditions and visualized the structure formation and subsequent rearrangement of PACl (flocculant made of aluminum hydroxide gel) and kaolinite flocs by visible light imaging. In a previous report, we analyzed the case of relatively low shear rate (G-value = 29 1/s) and confirmed that the flocculation process could be separated into two stages: a floc growth stage and a breakup/rearrangement stage. Once the large bulky flocs that reached the maximum size appeared, they rearranged and densified through structural fracture and rearrangement. In this report, this process was further investigated by conducting experiments under two different high shear rates (58 and 78 1/s) at which breakup and rearrangement became more pronounced, and three different aluminum kaolinite ratios (ALT ratios) that were over and under the optimum dosage (neutralization point by Zeta potential). Visualization results confirmed that, during the growth stage, the flocculation rate could be approximated by a scaling relationship between floc size and elapsed time, which depended on the ALT ratio. After reaching the maximum size, the floc rapidly became compact and dense following adsorption of the gel, incorporating fine fragments from erosion breakup. The over and under dosages created a lot of fragments of erosion breakup, but less so in the optimum dosage. In the optimum ALT ratio, fragments did not remain because they were incorporated into the flocs and densified, and the floc size was thought to be maintained. The floc circularity distribution peaked at around 0.6 and 1, suggesting that the flocs were spherical in shape due to erosion breakup.