A novel and effective preparation technology was developed to prepare ultrathin molybdenum disulfide (MoS2) crystals with a high yield of the top-down exfoliation. Multidimensional carbon nanotubes (MWCNTs) were selected to be an assistant to enhance the effect of the traditional ultrasonic exfoliation efficiency. The rough and messy tubes strengthened the shear force in some parts during the acoustic treatment, which helped to weaken the van der Waals force between the MoS2 layers. Excitingly, this high-efficiency strategy can increase the dispersion concentration of nanosheets by 15 times compared to the traditional acoustic production, which represented the preparation yield was improved greatly. It is found that the addition of MWCNTs not only facilitated the exfoliation efficiency of bulk material but also indirectly improved the adsorption of malachite green (MG) in wastewater. With a maximum removal capacity of 87.80 mg g−1, the adsorption ability of the nanotubes-reinforced layered adsorbent was effectively strengthened. In addition, the performance of reproducibility, stability, functioning free radical types, and the adsorption models were systematically studied.
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