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The convenient use of energy harvesting techniques has been a bottleneck issue in the rapid advancement of energy storage device technologies. [1] The energy harvesting approaches have witnessed several innovations in design and development in the process to attain miniaturization of devices with enhanced output efficiency. The concept of energy harvesting has its history in technological revolution with electromagnetic induction being an ideal concept in converting mechanical energy into electrical energy. [2,3] The incessant consumption of fossil fuels has led the technologists to ponder about alternate resources in energy consumption to develop distributed power supply and portable electronic devices with superior output performances. This led to the invention of triboelectric nanogenerators (TENGs) by Professor Z.L. Wang in 2012. [4] TENG is so far considered as the best option to harvest mechanical energy to consumable electrical energy for sensing and energy storage devices. TENG works on the combination of electrostatic induction and triboelectric effect. TENG enables the possibility to convert mechanical energy into electrical energy with the help of coupling effect between the electrostatic induction and contact electrification between the triboelectric materials, possessing different tendencies to gain or lose electrons. [5] This novel approach to harvest mechanical energy has the tendency to provide electricity for portable electronics and distributed power systems such as physiological monitoring, robotic systems, motion tracking, etc. The performance of TENG devices and TENG sensors has improved dramatically in the few years after its initial publication. [6][7][8] The friction effect is critical to the TENG's output performance, and altering the inner structure is the simplest and most cost-effective technique to increase the contact area without replacing the entire material. The variety of materials available for TENG production is huge, necessitating extensive study ahead of time to achieve the optimum results. [9] The proper selection of materials is vital for enhancing the triboelectric output of the TENG device. There are many techniques to fabricate triboelectric materials which include electrospinning, spin coating, etching, and 3D printing (3DP). [10] 3DP technology has emerged as a promising fabrication method for TENG development due to its fast production time, low-cost modeling, and simplicity of developing sophisticated and tailored structures with excellent material utilization efficiency. [11] The amalgamation of TENGs and 3DP has contributed to the encouragement of new-era energy harvesting technologies and self-powered sensing by making full use of their individual merits. The demerits of 3D printing (3DP) having lesser manufacturing precision than photoetching can be fulfilled by speedy layer-by-layer production of the complicated

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.