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Native defects can degrade the performance and stability of an optoelectric device. Herein, a zeolitic imidazolate framework-8 (ZIF-8)@H:ZnO core–shell nanorod arrays/Si heterojunction self-powered photodetector is demonstrated. Via the combined process of hydrogenation and ZIF-8 passivation, the photoresponsive characteristics of this photodetector could be significantly enhanced; the photodetector exhibited the superior detectivity of ∼2.14 × 1016 Jones (1 Jones = 1 cm Hz1/2 W−1), the high responsivity of ∼7.07 × 104 mA W−1, the prominent sensitivity of ∼2.08 × 1012 cm2 W−1 and broadband photodetection in the region ranging from ultraviolet to near infrared. As a critical figure of merit, its responsivity increased by nearly 5 orders of magnitude than that of the pristine ZnO nanorod arrays/Si heterojunction photodetector. More importantly, the comprehensive performance of the ZIF-8@H:ZnO core–shell nanorod arrays/Si heterojunction photodetector was significantly higher than that of ZnO-based photodetectors reported to date, and it was comparable to those of two-dimensional (2D) materials, zero-dimensional (0D) materials, topological insulators, perovskites and other oxide-based self-powered photodetectors. This novel post-treatment strategy has significant potential for application in the development of high-performance self-powered photodetectors. Moreover, this study may be extended to other oxide-based optoelectronic devices.