Cellulose nanomaterials have high strength and rigidity due to their highly ordered molecular structure, so they are expected to become the basic material for lightweight and high-performance man-made fibers. However, the use of pure nanocellulose to prepare high-performance fibrous filaments is still a challenge. This research successfully designed and demonstrated a microfluidic chip with self-twisting flow focusing. The chip enables the CNC to perform self-twisting in the process of forming a gel, increases the bond between the fibers, improves the mechanical properties of the fibers, and can efficiently and continuously produce highly ordered CNC fiber filaments. The prepared fiber filament has a tensile strength of 400 ± 20 MPa and a Young's modulus of 37.3 ± 3.8 GPa, which is the highest strength of the pure CNC fiber filament prepared at present. Its mechanical properties are also 150% higher than previously reported fiber filaments prepared by pure CNC.