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To further improve the output performance of triboelectric devices, reducing charge attenuation and loss has become a hot research topic. Particularly, textiles have emerged as one of the promising research directions for triboelectric devices owing to their special internal structure and large specific surface area. In the present work, polyacrylonitrile fibers are fabricated with two distinct structures to provide a higher dielectric constant due to the strong polar properties brought about by higher dipole moment of the CN group. In addition, the complex and closely connected structure of the textile increases specific internal surface area. As a friction layer, the output voltage is shown to increase to 625% of the initial value (from 8 to 60 V) after the application of friction for a short time due to accumulation property. When acting as a trapping layer, the charge loss after injection is effectively prevented due to excellent charge trapping effect. After 24 h, the triboelectric output performance remains at ≈70% of the initial value (decreasing from 320 to 220 V), which is more than 20 times that of the polytetrafluoroethylene film, which decreases from 125 to 19 V. The device is realized for the advanced application of multi‐modal sensors.

To build devices offering users comfortable experience, it is important to focus on form factor and multifunctionality. In this study, for the first time, multifunctional Zn clusters with shape memory, self‐healing, triboelectricity, and optical sensing synergized with rollable form factor are designed and fabricated by coordinating COO− and Zn2+. As pore forming agent, Zn clusters produce hierarchical porous structure depending on Zn amount. Zn clusters are applied as message transmitters and charge containers in optical sensing and corona charge injection, respectively. Moreover, Zn clusters in PVB‐COO‐Zn serve as positive tribomaterial due to Zn ion doping effect, increasing the output performance as the Zn amount reaches 20 wt%. In addition, injecting positive charge into PVB‐COO‐Zn 20 lead to more than 24 times increase in output performance compared to those of non‐porous structures. The reversibility of Zn clusters endows shape memory and self‐healing, synergized with the rollable form factor. The rollability is implemented using the long alkyl chain and the energy absorption of porous structure, providing damage resistance. The advancements in this work provide opportunities for multifunctional and unique applications (shape memory rotating‐triboelectric nanogenerator, rollable self‐healing touchpad, hidden tag) synergized with rollability that accomplishes working in broadened condition in near future.

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