Poly‐DADMAC Functionalized Polyethylene Oxide Composite Nanofibrous Mat as Highly Positive Material for Triboelectric Nanogenerators and Self‐Powered Pressure Sensors

Abstract The triboelectric nanogenerator (TENG) is a promising technology for self‐powered sensors and vibration‐driven energy harvesting, with its development especially influenced by the characteristics of tribomaterials. However, developing tribopositive materials with a strong cationic effect and high electron‐donating capability remains challenging. In this study, a novel polyethylene oxide@poly(diallyldimethylammonium chloride) (PEO@Poly‐DADMAC) composite nanofiber mat (NFM) is successfully fabricated using the electrospinning technique. It functions as a highly tribopositive material, particularly enhancing the performance of nanofiber‐based TENGs (NF‐TENGs). Through investigation of its physical and triboelectric properties, the study revealed that incorporating cationic Poly‐DADMAC with PEO effectively boosts NF‐TENG output by increasing the dielectric constant (twofold), electron‐donating affinities, and surface charge trapping capability. The fabricated NF‐TENG shows excellent output performance generating 980 V, a maximum power density of 5.6 Wm⁻², and an ultrahigh sensitivity of 8.923 V kPa⁻¹ which endows composite reliability for power supply and sensing capability. More importantly, the PEO@Poly‐DADMAC‐based self‐powered motion sensor with an NF‐TENG array is successfully demonstrated in multifunctional applications such as athlete activity tracking, and wireless gaming interface control. This study not only offers new insights into optimizing performance and selecting alternative tribomaterials but also provides valuable guidance for developing high‐output TENGs and highly sensitive self‐powered sensors.