Hysteresis effect greatly impacted performance and stability of perovskite solar cells. Ion migration and the resulting accumulation of interface ions were widely recognized as the most important origins. In this study, upconversion luminescent nanoparticles (UCNP) were used to modify the interface of the electron transport layer/perovskite active layer and the intrinsic perovskite active layer, and the effects of UCNP on the morphology, structure, spectral/optoelectronic properties, and ion migration kinetics of perovskite were systematically explored. The results indicated that the device with UCNP modified perovskite active layer has the best photoelectric conversion efficiency (PCE, 16.27%) and significantly improves the hysteresis factor (HF, 0.05). Furthermore, circuit switching transient optoelectronic technology was employed to investigate the ion migration kinetics without interference from photo-generated carriers, revealing the dual role of UCNP in suppressing ion migration and accumulation during the optoelectronic conversion process of perovskite solar cells. On the one hand, UCNP formed barrier layers that hinder ion accumulation. On the other hand, UCNP infiltrated into grain boundaries of perovskite phase during annealing, hindering ion migration and reducing the recovery voltage from 0.43 V to 0.28 V. The mechanism of carriers and ions interaction was explained based on the polarization-induced trap state model to declare the process of UCNP suppressing the hysteresis of perovskite photovoltaic devices. This work provides effective solution for regulating the hysteresis of perovskite solar cells.