LAUSR

Boosting output charge density is top priority for achieving high‐performance triboelectric nanogenerators (TENGs). The charge‐excitation strategy is demonstrated to be a superior approach to acquire high output charge density. Meanwhile, the molecular charge behaviors in the dielectric under a strong electric field from high charge density bring new physics that are worth exploring. Here, a rapid self‐polarization effect of a polar dielectric material by the superhigh electric field in a charge‐excitation TENG is reported, by which the permittivity of the polar dielectric material realizes self‐increase to a saturation, and thus enhances the output charge density. Consequently, an ultrahigh charge density of 3.53 mC m−2 is obtained with 7 µm homemade lead zirconate titanate−poly(vinylidene fluoride) composite film in the atmosphere with 5% relative humidity, which is the highest charge density for TENGs with high durability currently. This work provides new guidance for dielectric material optimization under charge excitation to boost the output performance of TENGs toward practical applications.