Although ferroelectric composites have been reported to enhance the performance of triboelectric (TE) devices, their performances are still limited owing to randomly dispersed particles. Herein, we introduce high-performance TE sensors (TESs) based on ferroelectric multilayer nanocomposites with alternating poly(vinylidenefluoride-co-trifluoroethylene) (PVDF-TrFE) and BaTiO3 (BTO) nanoparticle (NP) layers. The multilayers comprising alternating soft/hard layers can induce stress concentration and increase the effective stress-induced polarization and interfacial polarization between organic and inorganic materials, leading to a dielectric constant (17.06) that is higher than those of pure PVDF-TrFE films (13.9) and single PVDF-TrFE/BTO nanocomposites (15.9) at 10 kHz. As a result, the multilayered TESs with alternating BTO NP layers exhibit TE currents increased by 2.3 and 1.5 times compared to pure PVDF-TrFE without BTO NPs and PVDF-TrFE/BTO nanocomposites without multilayer structures, respectively. The multilayered TESs exhibit a high pressure sensitivity of 0.94 V/kPa (48.7 nA/kPa) and output power density of 29.4 mu Wcm(-2), enabling their application in the fabrication of highly sensitive healthcare monitoring devices and high-performance acoustic sensors. The suggested architecture of ferroelectric multilayer nanocomposites provides a robust platform for TE devices and self-powered wearable electronics.