chemical vapor deposition (CVD). When it comes to on-chip integrations, these strategies are limited by accessible materials and slow processing rate, [31] and the generated defects in the produced amorphous materials placed restrictions to its further applications in high-performance devices. [32] Therefore, novel approaches and methods of fabricating 3D micro/ nanostructures are highly demanded.Rolled-up nanotechnology is an alternative technique that fabricates 3D nanostructures out of planar films called nanomembranes. Nanomembranes are defined as planar thin films with thicknesses between one to a few hundred nanometers. [33] These nanomembrane materials behave like soft materials while maintaining excellent properties like their bulk counterpart and therefore is an ideal platform for fabricating 3D nanostructures. Inspired by concepts of origami and kirigami, [34][35][36][37] researchers folded and rolled these nanomembranes into a number of fascinating 3D structures. [17,[38][39][40][41][42][43][44] Several review articles have been published with emphasis on nanomembranes thinning and manufacture, mechanical deformation, fundamental studies, and their practical applications. [33,41,[45][46][47] By releasing strain-engineered planar functional nanomembranes on sacrificial layers, complex rolled-up structures including tubes, [48][49][50][51][52][53][54] rings, [54][55][56] and helices [42,[57][58][59] can be constructed (for instance, see Figure 1f). This approach can be applied to engineer a wide range of organic and inorganic materials and their combinations, including metals, insulators, traditional semiconductor families, and recently emerged 2D materials. Given its compatibility to standard CMOS fabrication process and ability to manufacture large periodic arrays with precise geometric control, rolled-up nanotechnology further expands the applications of 3D nanostructures to a number of areas, including optical resonators, [60,61] photodetectors, [62,63] micromotors, [64][65][66] energy storage, [67] drug delivery, [68] gas detection, [53] and environmental decontamination. [69] The versatility in the materials design and geometric tuning in rolled-up nanotechnology presents tremendous opportunities for further developing sophisticated 3D fine structures.In this review, we focus on the materials perspective and fabrication process of rolled-up nanotechnology. First, we give a brief introduction of rolled-up mechanism, as well as its fabrication techniques and control strategies. We summarize and highlight recent advances of different materials systems and their corresponding rolling methodologies. Second, Rolled-up nanotechnology is an appealing technique that tunes planar films into complex 3D fine structures. The rolling-up mechanism and methodology of a huge variety of materials and their combinations are summarized, including metals, insulators, traditional semiconductor families, polymers, and recently emerged 2D materials. The basic principles of strain induction, fabrication methods, and techni...