▎ 摘　　要

Graphene oxide (GO) has become a key component for high-performance carbon-based films or fibers based on its dispersibility and liquid crystallinity in an aqueous suspension. While the superior performance of GO-based fiber relies on their alignment at the submicrometer level, fine control of the microstructure is often hampered, in particular, under dynamic nature of GO-processing involving shear. Here, we systemically studied the structural variation of GO suspensions under shear conditions via in situ rheo-scattering and shear-polarized optical microscope analysis. The evolution of GO alignment under shear is indeed complex. However, we found that the shear-dependent structural equilibrium exists. GO showed a nonlinear structural transition with shear, yet there is a "universal" shear threshold for the best alignment, resulting in graphene fiber achieved an improvement in mechanical properties by similar to 54% without any chemical modification. This finding challenges the conventional concept that high shear stress is required for the good alignment of particles and their best performance.