<p>Perovskite light-emitting diodes (PeLEDs) fabricated through thermal evaporation are well suited for large-scale industrial production, owing to their compatibility with existing display panel manufacturing lines. However, the performance of all-evaporated PeLEDs lags behind that of their solution-processed counterparts, primarily due to the high defect density in evaporated perovskite films. Here we develop a sequential deposition combined with organic intercalation (SDOI) strategy to fabricate high-quality perovskite films by incorporating the multifunctional organic molecule phenformin hydrochloride (PFCl) into the perovskite crystallization process. The PFCl intercalation effectively prevents direct contact between the Cs and Pb precursors, thereby boosting the formation of reduced-dimensional perovskite films with highly uniform crystallographic orientation. Moreover, PFCl effectively passivates various types of defect, serving a dual role as both an organic spacer cation and a passivating agent. As a result, we demonstrate SDOI-based sky-blue PeLEDs with an external quantum efficiency of 20.12% and a maximum luminance of 23,704 cd m⁻². We also apply the SDOI strategy for the fabrication of high-performance green PeLEDs, demonstrating the method’s generality. Moreover, we integrate the SDOI-based all-evaporated PeLEDs into thin-film transistor-driven active-matrix display panels, demonstrating the potential of the SDOI strategy for display applications. Our SDOI strategy paves the way for efficient all-evaporated PeLEDs and their scaling up for practical applications.</p>