Despite many developed methods, it still remains a challenge to provide a simple and general strategy for the controlled preparation of chiral nanostructures. Here we report a facile and universal approach for the high-yield and scalable preparation of chiral nanofibers based on the self-assembly of various ultrathin one-dimensional and two-dimensional nanomaterials in vigorously stirred polymeric solutions. The obtained chiral nanofibers can be further transformed to same-handed chiral nanorings. As a proof-of-concept application, chiral MoS2 and multiwalled carbon nanotube nanofibers were used as promising active layers for flexible nonvolatile data storage devices. Impressively, the chiral MoS2 nanofiber-based memory device presents a typical nonvolatile flash memory effect with excellent reproducibility and good stability. Our method offers a general route for the preparation of various functional chiral nanostructures that might have wide applications.