Solvent‐Free Preparation of Ti ₃ C ₂ T x Nanoscrolls for Enhanced Nonlinear Circular Dichroism

One‐dimensional (1D) nanoscroll structure, formed by the curling of two‐dimensional (2D) nanosheet, holds significant application potential in electrical transport and nonlinear optics. However, conventional assisted rolling methods suffer from low curling efficiency or the introduction of additional organic solvents. Here, we report an interfacial energy driven self‐scrolling strategy for the fabrication of nanoscrolls. This approach enables the straightforward and efficient production of high‐quality 1D Ti 3 C 2 T x nanoscroll with ∼100% yield. Moreover, the applicability of this method extends to graphene oxide, showcasing its potential as a universal strategy for preparing 1D nanoscrolls from diverse 2D materials. 1D Ti 3 C 2 T x exhibits a second harmonic generation intensity approximately twice that of 2D Ti 3 C 2 T x and pronounced nonlinear circular dichroism (up to 0.55). These findings provide a platform for developing distinct 1D nanoscroll structures and demonstrate the potential for nanoscrolls in nonlinear optical devices.