atomic-scale (e.g., graphene, [12] MoS 2 [13] ), ultrathin nanomaterials exhibit outstanding mechanical, optical, and electrical properties. [6,10,14,15] Therefore, they have been attracting tremendous research interest in both academia and industries in recent years. Nonetheless, controlled manipulation of these ultrathin nanomaterials poses a general challenge to their applications. [16] To fabricate microor nano-devices, nanomaterials need to be purposely structured [16] and transferred [17,18] while any resultant deformation, such as the formation of curvatures and folds, [16] could change their electronic and photonic properties. On the other hand, because of their extremely low flexural rigidity, ultrathin nanomaterials can be easily deformed and/or even damaged by external stimuli (e.g., by solid-solid contacts). In addition, the presence of in-plane residual stress often leads to the rolling or twisting of ultrathin nanomaterials. [19,20] Therefore, it has never been straightforward to manipulate ultrathin nanomaterials in a controlled manner.Over the past years, tremendous efforts have been dedicated to structuring and manipulating ultrathin nanomaterials for real applications. According to the literature, [16,[21][22][23][24] the Ultrathin inorganic nanosheets (e.g., 2D nanomaterials, thin films, etc.) have attracted tremendous research interest because of their unique properties and promising applications. However, because of their ultrathin thickness (<100 nm) and low flexural rigidity, it is difficult to manufacture low-dimensional structures using these nanosheets. In this work, the observation of an intriguing elasto-capillary unfolding phenomenon is first reported which occurs on a variety of freestanding inorganic nanosheets floating on a liquid surface. Through theoretical modeling and experiments, it is demonstrated that one can easily unfold, re-roll, and transport different kinds of nanosheets by tuning the interfacial properties of the liquid. As a result, one can assemble nanosheets on the liquid surface into small structures (e.g., heterogeneous scrolls, optical resonators) and/or transfer them out of the liquid surface onto other surfaces for the manufacturing of flexible devices. The outcome of this research paves the way for nano-manufacturing of low-dimensional structures with ultrathin inorganic nanosheets.