Abstract Transition metal dichalcogenide nanoscrolls (NSs) exhibit unique optoelectronic properties due to their spiral tubular structures. In this study, we successfully fabricated WSe2 NSs with various morphologies, illustrating the evolution from planar to NS via an internal strain-driven rolling process. The anisotropic optical properties of the NSs were systematically analyzed by angle-resolve polarized Raman spectroscopy. For NSs with different rollup angles, the strain distribution is manifested by the variation of Raman intensity on the linear axis. In addition, the on/off ratio and detectivity of device based on bilayer NS reach 5.3 × 104 and 2.63 × 109 Jones, caused by the ultralow dark photocurrent. In summary, our study demonstrates a universal method for producing polymorphic products, demonstrating that bilayer WSe2 NSs hold significant potential as a platform for fundamental research and technological applications.