The mechanical properties of rodlike cellulose nanocrystals (CNCs) suggest great potential as bioderived reinforcement in (nano)composites. Poly(vinyl alcohol) (PVOH) is a useful industrial material and very compatible with CNC chemistry. High performance CNC/PVOH composite fibers were produced coaxial coagulation spinning, followed by hot-drawing. We showed that CNCs increase the alignment and crystallinity of PVOH, as well as providing direct reinforcement, leading to enhanced fiber strength and stiffness. At 40 wt % CNC loading, the strength and stiffness reached 880 MPa and 29.9 GPa, exceeding the properties of most other nanocellulose based composite fibers previously reported.