The rapid evolution of 3D‐printing (3DP) technologies has generated scope of developing advanced feedstock materials with excellent comprehensive properties. Material extrusion (ME) is one such 3DP technique with extensive range of commercial applications especially in aerospace applications. Herein, the current research focusses on developing ME‐based filaments with excellent functional characteristics by using polylactic acid (PLA) as the base polymer. The hybrid combination of carbon nanotubes and zinc oxide is synthesized by constructing a core–shell nanoparticles (CNS) which is then added into PLA under different wt%. The characterization techniques, such as X‐ray diffraction, Fourier‐transform infrared spectroscopy, scanning electron microscopy, transmission electron microscopy, etc., confirm the formation of CNS, which affirms to be an ideal reinforcement within PLA matrix. The mechanical properties of PLA are significantly enhanced with the tensile strength augmentation by 48.5% with only 0.2 wt% addition of CNS, while the thermogravimetric analysis results confirm the thermal stability enhancement for PLA/CNS composites. The fabricated PLA/CNS filaments display excellent flow characteristics as vindicated in rheological studies and ME‐printed prototypes exhibit refined output with exemplary finishing. The developed composite filaments can be harnessed as an advanced material in biomedical applications with exceptional properties.