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Hierarchically organized silica nanomaterials have shown great promise for nanomedicine. However, the synthesis of silica nanomaterials with a small size and macromolecular loading pore is still a big challenge. Herein, orderly curled silica nanosheets (OCSNs) with a ∼42 nm diameter and orderly connected large channels (∼13.4 nm) were successfully prepared for the first time. The key to the formation of the unique structure (OCSNs) is using an oil/water reaction system with high concentrations of the surfactant and alkali. The prepared