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The rapid development of state-of-the-art nanotechnology is driven by the emerging novel nanofabrication methods, such as self-rolling of 2D materials or nanosheets. Nonetheless, the traditional chemical etching-based "roll-up" technologies suffer from a low fabrication efficiency and generally produce only scroll-like structures. In this work, we develop a versatile, ultrafast, and etching-free method to synthesize self-rolled metallic nanostructures through hydrogel surface buckling enabled exfoliation, which enables rapid exfoliation an