Fundamental Material Parameters Governing the Performance of Polymer‐Based Triboelectric Touch Sensors

The growing demand for self‐powered electronics, such as touch sensors and wearable devices, highlights the need for reliable and efficient triboelectric systems. However, performance inconsistencies frequently originate from uncontrolled material morphology and processing conditions. This study explores the processing–structure–performance relationships in polymer‐based triboelectric systems, focusing on poly(vinylidene fluoride) (PVDF). Through controlled experiments incorporating auxiliary materials, poly(3‐hydroxybutyrate) (PHB) and carbon nanotubes (CNTs), and characterization via Differential Scanning Calorimetry (DSC), polarized optical microscopy (POM), Fourier transform infrared spectroscopy (FTIR), X‐ray diffraction (XRD), and scanning electron microscopy (SEM), we demonstrate that triboelectric performance is primarily driven by crystal size reduction rather than increased crystallinity. Additionally, optimized surface morphology, achieved through electrospinning, significantly enhances output by balancing fiber diameter and defect density. This work establishes a systematic framework for interpreting triboelectric behavior, emphasizes the need for standardization and morphological transparency, and provides guidelines for designing high‐performance devices via scalable fabrication methods.