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Efficient treatment of solutions and solid wastes containing Rhodamine B (RB), a common dye with potential carcinogenicity and sometimes used illegally in food industry, is of great importance because inappropriate treatment may lead to serious human and environmental risks. A novel nanomaterial, the mesoporous silica nanosheets prepared via electrospinning and calcination are applied to the adsorption of RB from aqueous solutions in this work. This sheet-like material is superior to classic powder adsorbents in recoverability, while good availability and stability favor its practical application. The effects of key parameters such as system pH, stirring rate, initial concentration, and contact time are studied. The adsorption isotherm type and the kinetic characteristic are analyzed. The results show that the mesoporous SiO2 nanosheets are efficient in removing RB from aqueous phase, presenting great potential to become a practical dye adsorbent. Regeneration experiments show that this novel adsorbent can be activated by ethanol extraction process. This study provides the academic field with a successful application case of nanostructured materials, which can be applied to a wider range of dyes similar to RB in physicochemical properties, showing prosperous value in advanced environmental purification.