In perovskite solar cells (PSCs), defective perovskite grain boundaries (GBs) and/or surface due to photo‐excitation and the resulted suboptimal carrier dynamics at the perovskite/charge transport layer, have largely limited further performance enhancement and aggravated the PSCs instability. Fundamentally preventing the formation of these trap‐states through a simple and efficient approach is thus critical to the enhancement of both device performance and stability. Herein, a novel semiconductive silicon naphthalocyanine derivative (Cl‐SiNcTI) to reduce the deep level trap states at the GBs and the surface of perovskite film is successfully employed via a newly proposed photon‐relaxation mechanism. The resulting benign p‐type surface polarity and suppressed non‐radiation recombination lead to improved charge transport in bulk perovskite and at the perovskite/spiro‐OMeTAD interface. With a synergistic contribution of the Cl‐SiNcTI and 2‐(2‐Fluorophenyl)ethylamine iodide (oFPEAI), a 24.30% efficiency is achieved in a single cell with excellent operational stability. Moreover, under steady‐state light illumination, 93% power output compared to its initial state can still be maintained after 250 h of continuous operation.

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A perovskite solar cell with DDQ doped spiro-OMeTAD HTL delivers a champion power conversion efficiency of 21.16%.