In this talk, it will be introduced that two allotropes of carbon nanomaterials can be assembled into high torsional strength fibers through rheological control. Two distinctive building blocks including graphene oxide (GO) and CNTs are spun in a coagulation bath to form hybrid fibers with highly oriented inner structures. CNTs and GO interact with each other and direct the structural manipulation. In addition, I introduce that a deformable MXene gel of well-defined multiscale structures can be prepared by self-assembly of sheets. By taking advantages of strong molecular interactions, mechanically strong fibers can be fabricated by drawing the MXene gel fibers. Due to its defect-free structure, MXene fiber has dense lamella, as well as a highly aligned multiscale structure. As an electrical wire, MXene fibers exhibite outstanding electrical conductivity and a high mechanical modulus, compared with other MXene-based assemblies.