photoelectric conversion efficiency (PCE) of ferroelectric PV devices since Nechache et al. have achieved the fabrication of Bi 2 FeCrO 6 -based PV devices with a record PCE of 8.1% in 2014. [4] Instead, most of the ferroelectric-based PV devices show a very low PCE (<1%) due to the wide bandgap (>3.0 eV) nature of ferroelectric materials. [5][6][7] The characteristics of wide bandgap and tunable PV effect in ferroelectric materials allow them to be suitably applicable in the field of self-powered ultraviolet (UV) photodetectors. [8,9] So far, self-powered photodetectors based on ferroelectric materials such as Pb(Zr,Ti)O 3 , [8,10] BaTiO 3 (BTO), [9] BiFeO 3 (BFO), [11,12] and 0.5Ba(Zr 0.2 Ti 0.8 )O 3 -0.5(Ba 0.7 Ca 0.3 )TiO 3 (BZT-BCT) [13] have been reported, which open prospects for applying ferroelectric materials in fields such as environmental monitoring, biomedicine, and missile tracking. [14][15][16] For ferroelectric-based self-powered UV photodetectors, the ferroelectric depolarization electric field (E dp ) and the built-in electric field at the ferroelectric/electrode interface are the main driven force of photogenerated carriers. [6,17,18] However, the device performance of so far reported ferroelectric-based self-powered UV photodetectors is yet inferior, owing to the limited photogenerated carriers separation ability of ferroelectric depolarization electric field. [17] For example, responsivities (R) of these detectors are on the order of 10 −7 -10 −4 A W −1 , which are much lower than those of the semiconductor-based detectors. [17,[19][20][21][22][23] Thus, it's highly demanding to further optimize the device performance of ferroelectric-based self-powered UV detectors. In ferroelectric-based solar cells, the device performance can be effectively improved by combining ferroelectric materials with various semiconductor materials, such as ZnO, [24][25][26] CuO, [27] and NiO, [28] to construct ferroelectricsemiconductor heterojunctions. For example, Wu et al. fabricated a FTO/BFO/ZnO nanorods/PEDOT:PSS/Au device, which showed a photocurrent by over 64 times larger than that of a similar device without the ZnO nanorods. [24] The significantly enhanced photocurrent could be attributed to the improved efficiency of carriers transportation and charge collection resulted from the introduction of ZnO nanorods. Ferroelectric materials have aroused increasing interest in the field of self-powered ultraviolet (UV) photodetectors for their polarization electric field induced photovoltaic (PV) effect. However, the device performance of currently reported ferroelectric-based self-powered UV detectors remains to be improved. Herein, achievement of high-performance ZnO/ Pb 0.95 La 0.05 Zr 0.54 Ti 0.46 O 3 (PLZT) heterojunction-based self-powered UV photodetectors is demonstrated by coupling the ferroelectric depolarization electric field (E dp ) and built-in electric field (E ZnO/PLZT ) at the ZnO/PLZT interface with a II-type energy band alignment. The ZnO/PLZT heterojunction-based self-powered UV photodetector...