The 3D printing technique has recently become more prevalent among researchers for the fabrication of nanocomposites. The low crystallinity of polylactic acid (PLA) leads to the poor mechanical and thermal properties of its 3D-printed products, which restrict their applications in many fields. To overcome the limitations of PLA, the present work aims to develop PLA-based bionanocomposite filaments with varying percentages (1, 3, and 5 wt%) of crystalline nanocellulose (CNC) through a single screw extruder. The filaments will be further utilized for the development of bionanocomposite samples to evaluate their properties. The effect of CNC reinforcement on the chemical structure of the filaments was analyzed by FTIR analysis. XRD analysis revealed that the crystallinity of the filaments was significantly improved due to the nucleating effect of CNC. The maximum crystallinity was observed in the filament containing 1 wt% CNC, which was 26% higher than the pure PLA filament. The thermal and mechanical performance of the filaments was also considerably improved after CNC reinforcement, which was confirmed by DSC-TGA and tensile test analysis. The maximum tensile strength and tensile modulus were observed to be 48.9 MPa and 1700 MPa, respectively, in the filament reinforced with 1 wt% CNC, which was 35.5% and 21.89%, respectively, higher than those of the pure PLA filament. Rheological analysis showed that the complex viscosity, storage modulus, and loss modulus of the filaments were significantly affected by the reinforcement of CNC.